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Metal–Organic Frameworks Derived Functional Materials for Electrochemical Energy Storage and Conversion: A Mini Review

Cite this: Nano Lett. 2021, 21, 4, 1555–1565
Publication Date (Web):February 10, 2021
https://doi.org/10.1021/acs.nanolett.0c04898

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Abstract

With many apparent advantages including high surface area, tunable pore sizes and topologies, and diverse periodic organic–inorganic ingredients, metal–organic frameworks (MOFs) have been identified as versatile precursors or sacrificial templates for preparing functional materials as advanced electrodes or high-efficiency catalysts for electrochemical energy storage and conversion (EESC). In this Mini Review, we first briefly summarize the material design strategies to show the rich possibilities of the chemical compositions and physical structures of MOFs derivatives. We next highlight the latest advances focusing on the composition/structure/performance relationship and discuss their practical applications in various EESC systems, such as supercapacitors, rechargeable batteries, fuel cells, water electrolyzers, and carbon dioxide/nitrogen reduction reactions. Finally, we provide some of our own insights into the major challenges and prospective solutions of MOF-derived functional materials for EESC, hoping to shed some light on the future development of this highly exciting field.

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1. Introduction

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Electrochemical energy storage and conversion (EESC) technologies have been recognized as the most practical options to mitigate the ever-growing energy crisis and environmental disruption in view of their high energy efficiency and low environmental impact. (1−3) Currently, the most studied and relatively mature EESC systems include supercapacitors (SCs), rechargeable batteries, fuel cells, water electrolyzers, and carbon dioxide/nitrogen reduction reactions (CO2RR/NRR). The first two are the major energy storage systems in which advanced electrodes with high specific capacity and durability are highly desired. (4−7) The latter three are the forefront energy conversion systems in which functional electrocatalysts with high activity, stability, and selectivity are urgently needed. (8−11) Despite the different working principles, these electrochemical systems all have the ultimate pursuit for the physicochemical properties of materials (for example, high specific surface area, excellent electronic conductivity, well-defined redox couples, superior electrocatalytic activity and selectivity, long-term stability, etc.), which determine their final storage capacity and conversion efficiency in EESC devices. (3,12−14) Therefore, seeking novel functional materials with the desired composition and structure has always been the top priority for the development/breakthrough of future EESC technologies.
Metal–organic frameworks (MOFs) are a new class of porous materials with high crystallinity and long-range order, which are interconnected by the coordination bonds of metal ions/clusters and organic ligands. (9) Compared with pristine MOFs and MOF composites, MOF derivatives possess higher chemical stability, electronic conductivity, and electrochemical performance thus have drawn deep and increasing interest in various EESC systems, as witnessed by a large number of publications in the past decades. (7,8,15−17) Although the insufficient electronic conductivity and relatively poor chemical stability seriously hinder MOFs’ wide applications in electrochemical systems, their size, morphology, structure, and other features can be well inherited and preserved in the derivatives by rational design and synthesis. (9,18) Moreover, the abundant inorganic units and organic linkers, as well as their high surface area and porosity with rational pore-size distribution, grant more possibilities in structure and composition of porous functional materials derived from MOFs for EESC. (18−20) For example, when used as electrodes for SCs and various batteries, the hollow micro/nanostructures derived from MOFs can effectively adapt to the large volume expansion during the charging/discharging processes. (13,14) As electrocatalysts for various energy conversion systems, MOF-derived hierarchical carbon-based hybrid structures can not only facilitate the charge/ion transfer but also expose more active sites for the reactive species adsorption and subsequent electrocatalytic reactions. (21,22) Although several early reviews have summarized MOF-based functional materials and their energy applications, most of them focus on a certain aspect of synthesis strategy, composition, structure, energy storage, or conversion applications. (8,9,19,23−25) Given the rapid progress of MOF-derived materials and various EESC technologies, a short but comprehensive review summarizing the latest progresses and breakthroughs will be useful for their future developments in various high-efficiency EESC systems.
In this Mini Review, we aim to provide an up-to-date overview of the investigations on the applications of MOF-derived functional materials in EESC systems. We first briefly introduce the synthetic strategies for MOF-derived materials based on their composition, structure, and performance improvement. Thereafter, we highlight some of the latest advances in engineering MOF-derived functional materials as advanced electrodes or high-efficiency electrocatalysts for EESC devices. Specifically, we categorize our discussion in terms of the following: (i) synthesis strategies for SC electrodes; (ii) hollow transition metal oxides (TMOs), chalcogenides (TMCs) and hydroxides as cathodes or anodes for lithium-ion/sodium-ion/lithium–sulfur batteries (LIBs/SIBs/LSBs), respectively; (iii) atomic site electrocatalysts as cathodes for metal-air batteries (MABs) and fuel cells; (iv) porous transition metal compound hybrid structures for water electrolysis involving hydrogen/oxygen evolution reactions (HER/OER) over a full pH range; (v) porous carbon-based electrocatalysts for CO2RR and NRR. Finally, this Mini Review concludes with some of our own insights into the current major hurdles and their prospective solutions, hoping to stimulate continuous innovations for advancing MOF-derived functional materials for various EESC technologies.

2. Synthesis Strategies for MOF Derivatives and Their Composition, Structure, and Performance Regulation

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Generally speaking, the synthesis process of MOF-derived materials involves two steps, the design and fabrication of MOF-based precursors and deliberate post-treatments. Herein, the MOF-based precursors include pristine MOFs and MOF composites. The former is mainly prepared by selecting the appropriate metal source, organic ligand, and solvent through solvothermal methods, (9,26) and the latter can be obtained by impregnation with guest species, blending assembly, surface coating/growth, electrodeposition, electrospinning, and even mechanical mixing. (13,16) By contrast, the post-treatment process and condition of these MOF-based precursors almost determine the final morphology, structure, and composition of the derivatives, which in turn determine the electrochemical performance. (13,15) Therefore, much more effort has been devoted to exploring and developing new conversion strategies. The thermal and chemical instability of MOFs points to two mainstream postprocessing strategies, namely high-temperature pyrolysis and wet chemical reaction. On the basis of the different conversion mechanisms during the postprocessing, the strategies can be summarized as four categories: (i) self-pyrolysis under inert atmosphere, (27,28) (ii) gas-phase chemical reactions, (29,30) (iii) liquid-phase chemical reactions, (31,32) and (iv) chemical reactions combined with heat treatments. (33,34) By virtue of tuning the size, morphology, structure, and composition of MOF precursors and deliberately manipulating the conversion process, various compositions (carbons, metal/carbons, metal compounds/carbons, metal compounds) and structures (porous, yolk–shell, hollow, frame, hierarchical, etc.) from zero to three dimensions have been obtained in the MOF derivatives. Besides, to meet the requirements for some specific EESC systems, various approaches for surface/interface modulations, such as support interaction, (27,35) defect/doping, (34,36) surface modification, (37) heterostructure, (28,35) and so forth, have been developed, which can induce novel physicochemical properties and strong synergistic effects to greatly enhance the electrochemical performance. Owing to these intriguing compositional and structural features, these MOF-derived functional materials show great application prospects in various EESC systems. Figure 1 shows the overview of the synthetic strategy, composition, structure, and performance improvement approaches of MOF-derived functional materials in various EESC applications.

Figure 1

Figure 1. Synthetic strategies of MOF-derived functional materials with different compositions and structures, performance improvement approaches, and their applications in various EESC systems.

3. Applications in Various EESC Systems

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SCs

SCs have received widespread attention in the field of energy storage owing to their safe and fast charging/discharging characteristics, nevertheless, the relatively low energy density largely limits their widespread application. (38) Regarding the electric double layer capacitance or pseudocapacitance mechanism, the most promising approach for improving the energy density is to design and synthesize advanced electrodes with high porosity and electric conductivity, as well as abundant redox couples. (24,39) A growing number of works about MOF derivatives toward SCs have been done during the past few years, including some recent reviews about MOFs and/or MOF derivatives. (17,19,24,38,40) Therefore, we herein briefly introduce some typical synthetic strategies toward high-performance electrodes with unique nanoarchitectures. For example, Hu et al. reported three types of CoS nanoboxes (NBs) with different subunits by delicately manipulating the chemical reactions of Co-based zeolitic imidazolate framework (ZIF-67) with water and Na2S (Figure 2a). (41) Chen et al. carbonized the Zn-based zeolitic imidazolate framework (ZIF-8)/polyacrylonitrile (PAN) matrix obtained by electrospinning to obtain interconnected hollow nanoparticles (NPs)-based N-doped carbon nanofibers (Figure 2b). (42) Guan et al. developed a general method to prepare highly complex multishelled mixed TMO particles by a subsequent thermal treatment of amorphous coordination polymers (Figure 2c). (43) Lu et al. recently prepared CoO/Co–Cu–S hierarchical tubular heterostructures (HTHSs) by a facile chemical transformation of electrospinning PAN-Co(CH3COO)2/Cu(NO3)2 nanofibers (Figure 2d). The unique HTHSs and synergy between the two components endow the CoO/Co–Cu–S HTHSs-based hybrid SC device with high energy density and long-cycling stability. (35)

Figure 2

Figure 2. Some typical synthesis strategies of MOF-derived functional materials for SCs. (a) Sequentially modulate the chemical reactions of ZIF-67 with water and Na2S to prepare complex CoS NBs. Reprinted with permission from ref (41). Copyright 2016, Elsevier B.V. (b) Electrospinning followed by carbonization for hollow NPs-based N-doped carbon nanofibers. Reprinted with permission from ref (42). Copyright 2017, Royal Society of Chemistry. (c) Subsequent thermal treatment toward multishelled metal oxide particles. Reprinted with permission from ref (43). Copyright 2017, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) Multistep approach to CoO/Co–Cu–S HTHSs. Reprinted with permission from ref (35). Copyright 2019, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

LIBs

Among various rechargeable batteries, LIBs have been the predominant power source for daily portable electronic devices. However, conventional LIBs constructed with a graphite anode and a lithiated TMO cathode are approaching a practical upper limit. (4) Therefore, an enormous amount of effort has been focused on searching for alternative electrode materials with novel compositions and unique structures hoping to provide higher capacity and better rate capability. Encouragingly, MOFs provide us great opportunities to design and synthesize novel electrode materials, especially for TMO-based hollow structures, by using them as precursors or templates. (13,44) For example, triple-shelled Co3O4@Co3V2O8 NBs have been reported by Lu et al. through the solvothermal reaction between ZIF-67 with vanadium oxytriisopropoxide followed by thermal annealing in air (Figure 3a). (45) Recently, Huang et al. prepared an elegant hybrid structure consisting of ultrafine Co3O4 hollow NPs evenly embedded in mesoporous walls of carbon NBs (H–Co3O4@MCNBs) by a facile MOF-engaged etching-pyrolysis-oxidation strategy. Hollow NPs uniformly confined in the carbon wall of NBs can be observed by a typical transmission electron microscopy (TEM) image (Figure 3b), and the discharge–charge voltage curves at different current densities indicate the outstanding rate capability (Figure 3c). (44) In addition to TMOs, MOF-derived TMCs, (46,47) phosphides (TMPs), (48) nitrides, (49) and so forth have also been reported as anodes for LIBs. It is worth mentioning that a few MOF derivatives are also used as cathodes for LIBs. As a proof of concept, Lin et al. recently reported a binder-free LiCoO2 cathode by pyrolysis of Li-doped ZIF-67. (50)

Figure 3

Figure 3. MOF-derived hollow structures for various rechargeable batteries. (a) TEM image of a triple-shelled Co3O4@Co3V2O8 NB. Reprinted with permission from ref (45). Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) TEM image and (c) discharge–charge voltage profiles at various current densities of H–Co3O4@MCNBs for lithium storage. Reprinted with permission from ref (44). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) TEM image of a Cu-CoSe2 microbox. Reprinted with permission from ref (31). Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) TEM image and (f) discharge–charge voltage profiles at various current densities of Cu-CoS2@CuxS NBs for sodium storage. Reprinted with permission from ref (32). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (g) TEM image of double-shelled CH@LDH nanocages. Reprinted with permission from ref (65). Copyright 2016, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (h) TEM image of a hollow Ni/Fe LDH polyhedron and (i) discharge–charge voltage profiles at various current densities as a sulfur host for LSBs. Reprinted with permission from ref (66). Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

SIBs

With the increasing concerns of the cost and limited lithium reserve, SIBs that possess a similar working mechanism to LIBs have received much interest as a promising alternative to LIBs for grid-scale energy storage. (51) However, the higher reduction potential and much larger ionic radius of Na+ than Li+ lead to sluggish kinetics and extensive volume changes in the electrode materials during sodiation/desodiation processes. (5) Among various porous materials, MOF derivatives have shown great advantages in constructing versatile electrode materials, such as carbon, (52) metals, (53) TMPs, (54) TMOs, (55) TMCs, (31,32,56) as well as their composites, (57) for high-performance SIBs. For example, Wang et al. synthesized CoS2 multishelled NBs with precisely controlled two to five shells for sodium storage by an “ion-conversion-exchange” strategy. (56) Fang et al. used Co–Co Prussian blue analogue (PBA) microcubes as the starting material to obtain hierarchical Cu-doped CoSe2 (Cu-CoSe2) microboxes assembled by ultrathin nanosheets (NSs) through a two-step ion-exchange method (Figure 3d). As expected, these hierarchical Cu-CoSe2 microboxes exhibit good rate capability and cycling performance toward sodium storage. (31) Recently, they also synthesized an integrated nanostructure composed of copper-substituted CoS2@CuxS double-shelled NBs (Cu-CoS2@CuxS DSNBs) through a sequential anion and cation exchange reaction by using ZIF-67@ZIF-8 core–shell nanocubes as precursors (Figure 3e). Benefiting from the unique shell configuration and complex composition, the Cu-CoS2@CuxS DSNBs show outstanding rate capability with a capacity of 515 and 333 mAh g–1 at a current density of 0.1 and 5.0 A g–1, respectively (Figure 3f). (32) Similar to the fact that fewer MOF derivatives are reported as cathodes for LIBs, there are also relatively few works of MOF derivatives as cathodes for SIBs. (58) Nonetheless, it is worth noting that MOF-derived carbon-based materials are increasingly used as anodes for potassium-ion batteries, another promising alternative to LIBs. (59)

LSBs

Developing advanced host materials for sulfur to effectively trap the intermediate products is of great importance for designing high-performance LSBs, which can efficiently avoid the low Coulombic efficiency and self-discharge behavior. (60) Porous carbon materials have been actively explored as host materials for LSBs due to their large surface area, high porosity, and good electrical conductivity. (61) However, due to the repulsion between the polar polysulfides and the nonpolar carbon hosts, these carbon/sulfur composite cathodes usually decay rapidly especially when the sulfur content reaches about 70 wt % or above. To solve these obstacles, Lou’s group has designed a series of hollow structures containing polar TMOs/TMCs/nitrides/hydroxides as hosts to provide both physical barriers and chemical sorption for intermediate polysulfide products. (62−66) For example, Zhang et al. successively designed and prepared double-shelled hollow structures of cobalt hydroxide and layered double hydroxides (CH@LDH) (Figure 3g), hollow Ni/Fe LDH polyhedrons (Figure 3h) as advanced sulfur hosts to enhance the performance of LSBs even when the sulfur content exceeds 70 wt %. (65,66) Thanks to the abundant sulfiphilic groups of LDHs and the hollow architecture, the obtained S@Ni/Fe-LDH cathode delivered a high rate capability (Figure 3i). (66) In view of the higher electrical conductivity of selenium than sulfur and the limited Li reserve, other alkali metal-chalcogen batteries, such as Li–Se, Li–SexSy, Na–S, Na–Se, K–S, and K–Se batteries have emerged and achieved some initial success by using MOF-derived porous materials as cathode hosts. (63,67) For example, Song et al. reported a ZIF-8@ZIF-67-derived hierarchical nitrogen-doped porous carbon (NPC) core–shell structure for effectively confining Se for high-performance Li–Se batteries. (68) Zhang et al. recently utilized a MOF-derived Co-containing NPC as a catalytic sulfur cathode host for Na–S batteries. (69) Zhou et al. designed N and O dual-doped porous carbon nanocages anchored with carbon nanotubes to confine active Se for high-performance K–Se batteries. (70)

MABs

Rechargeable MABs consist of a metal anode (e.g., Li, Mg, Al, Zn, and so forth), electrolyte (aqueous or nonaqueous), and an air cathode absorbing the surrounding air. (6)Figure 4a shows the typical configuration and discharge–charge process of alkaline aqueous Zn-air batteries (ZABs), which have received the most favorable consideration due to their remarkable advantages such as high theoretical energy density, low capital cost, flatter operating voltage, high operation safety, and environmental benignity. (71) As the critical component for rechargeable ZABs, various bifunctional oxygen electrocatalysts derived from MOFs have been reported as air cathodes to facilitate the oxygen reduction reaction (ORR) and OER. (9,10,72) Impressively, various strategies involving MOFs have been developed to prepare atomic site electrocatalysts as highly efficient air cathodes for ZABs due to their maximum atomic utilization efficiency and distinct active sites with high catalytic activity, stability, and selectivity. (11,73) For example, Yang et al. reported a universal high-temperature gas-transport strategy to directly transform various TMOs into isolated single-atom sites (ISAS) onto the ZIF-8-derived NPC supports. The high-angle annular dark-field scanning transmission electron microscope (HAADF-STEM) image and corresponding energy-dispersive X-ray spectroscopy (EDS) mappings confirm the obtained Cu ISAS/NPC catalyst (Figure 4b), which exhibits a maximum power density of 280 mW cm–2 in ZAB, superior to Pt/C-based ZAB (Figure 4c). (30) Very recently, Chen et al. synthesized a MOF-derived Co single-atom catalyst (SAC) with the optimal Co1–N3PS active moiety incorporated in hollow carbon polyhedron (Co1–N3PS/HC). The HAADF-STEM image and corresponding EDS mappings show the uniform atomic dispersion of Co, C, N, P, S elements (Figure 4d). The maximum power density of the Co1–N3PS/HC-based ZAB reaches 176 mW cm–2, higher than that of Pt/C-based ZAB (Figure 4e). (74) In addition to these SACs, MOF-derived metal-free carbons, metal compounds, and their mixtures have also been reported as ORR electrocatalysts for MABs and summarized well in some important reviews. (6,8,9,75)

Figure 4

Figure 4. MOF-derived atomic site electrocatalysts for alkaline ZABs and acidic PEMFCs. (a) Configuration and discharge–charge process of a typical ZAB. (b) HAADF-STEM image and corresponding EDS mapping images of Cu ISAS/NC, (c) discharge polarization and corresponding power density plots of Cu ISAS/NC based ZABs. Reprinted with permission from ref (30). Copyright 2019, Springer Nature, licensed under a Creative Commons Attribution (CC BY) license: http://creativecommons.org/licenses/by/4.0/. No changes were made. (d) HAADF-STEM image and corresponding EDS mapping images of Co1–N3PS/HC, (e) discharge polarization and corresponding power density plots of Co1–N3PS/HC based ZABs. Reprinted with permission from ref (74). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) Schematic illustration of a typical PEMFC. (g) MAADF-STEM image of 20Mn-NC-second catalyst, and (h) fuel cell performance of the best-performing 20Mn-NC-second and 20Fe-NC-second catalysts in both H2/O2 and H2/air conditions. Reprinted with permission from ref (33). Copyright 2018, Springer Nature. (i) HAADF-STEM image of Fe/Ni–Nx/OC, and (j) discharge polarization curves and the corresponding power density plots of PEMFC with Fe/Ni–Nx/OC as cathode using H2/O2 and H2/air as fuels. Reprinted with permission from ref (81). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fuel Cells

Compared with direct alcohol fuel cells and alkaline anion exchange membrane fuel cells, proton-exchange membrane fuel cells (PEMFCs) using hydrogen as the fuel merit high power density, quick start-up, and low operating temperature and have been actively developed to power human society. (76)Figure 4f shows the configuration and schematic diagram of a typical PEMFC. However, the sluggish cathodic ORR process and the scarcity of expensive Pt greatly hinder their wide application. As illustrated in the MABs part, transition metal (Mn, Fe, Co, Ni, etc.) and nonmetal (mainly N) heteroatom-coordinated carbons (denoted as M–N–C) have shown outstanding ORR performance and thus been explored as promising platinum-group-metal-free (PGM-free) catalysts to boost ORR in PEMFCs. The diverse metal elements and organic ligands in MOFs offer a new paradigm for designing PGM-free (especially M–N–C) catalysts at a molecular level. (73,77) Wu’s research team has achieved exciting results about M–N-C catalysts as cathodes for PEMFCs in the past three years. (33,78−80) For example, they prepared a Mn–N–C catalyst with high-density MnN4 sites through a two-step doping and adsorption approach by using Mn-doped ZIF-8 as precursors. The bright spots shown in the high-resolution medium-angle annular dark-field (MAADF)-STEM image indicate a high density of Mn doping (Figure 4g). The optimized 20Mn-NC-second catalyst (where 20 is the molar percentage of Mn against the total metals in solutions during the synthesis of Mn-doped ZIF-8; second refers to the sample obtained after the second adsorption step) exhibits high current densities of 0.35 and 2.0 A cm–2 at 0.6 and 0.2 V, respectively in PEMFCs under H2/O2 condition (Figure 4h). (33) Recently, double-metal active sites are designed to further improve the ORR performance of SACs in PEMFCs. Most recently, an atomically dispersed Fe and Ni catalyst coanchored to a microsized N-doped graphitic carbon support with unique trimodal-porous structure and highly ordered macropores (denoted as Fe/Ni–Nx/OC) (Figure 4i) is reported by a template method combined with wet-chemistry metal-ion impregnation and pyrolysis. Because of its high ORR activity, a PEMFC based on the Fe/Ni–Nx/OC cathode exhibits a maximum power density of 580 and 210 mW cm–2 under H2–O2 and H2–air condition, respectively, both at a 1.0 bar pressure (Figure 4j). (81)

Water Electrolysis

Electrochemical water splitting for hydrogen generation from renewable energy resources has been considered as a green and efficient strategy to achieve a carbon-neutral future. (11,82) Recently, numerous MOF-derived functional materials have been reported as electrocatalysts to lower the overpotentials for HER and OER, two of the crucial half reactions for water splitting. (8,25) Compared with SACs, metal compounds have more metallic active sites for HER/OER, thus we herein briefly highlight some recent breakthroughs in engineering MOF-derived metal compounds toward high-efficiency water splitting, taking into account the synthesis strategies, catalyst composition/structure/reconstruction, electrolyte pH, and device configuration. For example, Lu et al. reported a universal and effective route for highly crystalline TMP hollow structures through the etching and coordination reaction between different MOFs and phytic acid, followed by a calcination process. Benefiting from the hollow structure and electronic regulation by cationic dopant, the obtained Ni-doped FeP/C (NFP/C) catalysts show superior activity for HER over the full pH range (Figure 5a–c). (34) Recently, the same group reported a series of hierarchical hollow nanoplates (HHNPs) composed of ultrathin Co3O4 NSs doped with 13 different metal atoms by a cooperative etching-coordination–reorganization approach, among which the obtained Fe-doped Co3O4 HHNPs manifest a huge improvement in overpotential for OER in 1.0 M KOH (Figure 5d–f). (83) Also, Lou and co-workers have also developed novel strategies for other MOF-derived metal compounds for HER/OER, such as Co–Fe mixed oxides with nanocuboid-assembled framelike superstructures, (29) Ni–Fe mixed diselenide nanocages, (84) Co3O4/Co–Fe oxide double-shelled NBs, (85) ultrafine dual-phased carbide nanocrystals confined in porous N-doped carbon dodecahedrons, (86) iron–cobalt (oxy)phosphide NBs, (87) and double-shelled Ni–Fe LDH nanocages. (88)

Figure 5

Figure 5. MOF-derived metal compound-based electrocatalysts for water splitting. (a) Schematic illustration, (b) TEM image, and (c) polarization curves in 0.5 M H2SO4 for HER of NFP/C hollow nanorods. Reprinted with permission from ref (34). Copyright 2019, American Association for the Advancement of Science (AAAS), distributed under a Creative Commons Attribution-NonCommercial international (CC BY-NC) license. http://creativecommons.org/licenses/by-nc/4.0/. The Authors, some rights reserved; exclusive licensee AAAS. (d) Schematic illustration, (e) TEM image, and (f) polarization curves in 1.0 M KOH for OER of Fe–Co3O4 HHNPs. Reprinted with permission from ref (83). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, licensed under a Creative Commons Attribution (CC BY) license: http://creativecommons.org/licenses/by/4.0/. We have rearranged the position of “Etching/adsorption” and moved the image representing the enlarged nanosheet from the original label location. (g) Schematic illustration, (h) AC-HAADF-STEM image, and (i) polarization curves in a broad pH range of 0–14 for OER (inset: corresponding voltages at 10 mA cm–2) of RuIrOx nanonetcages. Reprinted with permission from ref (91). Copyright 2020, Springer Nature, licensed under a Creative Commons Attribution (CC BY) license: http://creativecommons.org/licenses/by/4.0/. We have moved the “Dispersing”, “Etching”, and “Holing” from the original label locations. (j) Schematic illustration, (k) TEM image, and (l) polarization curves in 1.0 M KOH with and without 10 mM HMF in an H-type cell (inset) of MoO2–FeP@C porous nanospindles. Reprinted with permission from ref (92). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Compared with single-function electrocatalysts aiming at only HER or OER under a particular electrolyte condition, bifunctional catalysts possessing pH-universal compatibility are more appreciated in practical applications, so that different electrolytes, even wastewater and seawater can be directly used for hydrogen production, thereby improving operational reliability and reducing costs. (89,90) Recently, Zhuang et al. developed a dispersing-etching-holing strategy for preparing a three-dimensional (3D) open nanonetcage RuIrOx (x ≥ 0) catalyst (Figure 5g). Because of the unique highly porous architecture assembled by interconnecting ultrathin nanowires as shown by the aberration-corrected HAADF-STEM (AC-HAADF-STEM) in Figure 5h, the RuIrOx nanonetcages achieved high-performance overall water splitting over a full pH range with a potential of 1.45 V (pH = 0) or 1.47 V (pH = 14) versus the reversible hydrogen electrode (RHE) at 10 mA cm–2 (Figure 5i). (91) Nonetheless, the efficiency of water splitting is severely hampered by the sluggish kinetics of anodic OER process. To solve these obstacles, a new strategy of substituting the OER by some thermodynamically favorable oxidation reaction of small organic molecules, such as hydrazine, urea, amine, alcohols, 5-hydroxymethylfurfural (HMF), furfural, and so forth, has been developed to improve the efficiency of water splitting for hydrogen production. (82) As a proof of concept, Yang et al. proposed a porous carbon-encapsulated MoO2–FeP heterojunction (MoO2–FeP@C), which is formed by in situ growth of phosphomolybdic acid and iron-based complex (PMo12@Fe complex) onto FeOOH, followed by a low-temperature phosphorization (Figure 5j,k). Benefiting from the interfacial electronic structure, the voltage at 10 mA cm–2 of a two-electrode alkaline electrolyzer employing MoO2–FeP@C as both the anode and cathode noticeably reduces from 1.592 V for pure water splitting to 1.486 V with the addition of 10 mM HMF (Figure 5l). (92)

CO2RR and NRR

Electrochemical CO2RR to produce carbon monoxide, formic acid, formaldehyde, methanol, ethanol, methane, and so forth is an effective approach to alleviate global warming and energy issues. (93−95) However, due to its complexity with multistep reactions of protons and electrons, as well as competitive HER, highly active and selective electrocatalysts are highly desired. Recently, MOF-derived SACs, metal/alloy, and TMOs have been studied as active and selective electrocatalysts toward CO2RR. (96,97) For example, the Wu and Li group has adopted MOFs to assist in the preparation of a series of Co or Ni SACs for efficient CO2RR to yield CO. (98−101) NPC with a high concentration of active N (pyridinic and graphitic N) was also reported by Ye et al. as a highly efficient electrocatalyst toward CO2RR to CO with a record Faradaic efficiency (FE) of 98.4% at −0.55 V versus RHE among the reported NPC electrocatalysts. (102) Also, Zhu et al. (103) and Deng et al. (104) reported MOF-derived 3D hierarchical Cu dendrites and Bi2O3@C porous nanorods, respectively. When used as the electrocatalysts for CO2RR, the former demonstrates a high current density of 102.1 mA cm–2 with a selectivity of 98.2% for formate in an ionic-liquid-based electrolyte and a commonly used H-type cell; the latter exhibits a partial current density of over 200 mA cm–2 with a stable and high FE of 93% toward formate in a flow cell configuration. Very recently, electrocatalytic NRR for NH3 production from N2 and H2O at ambient conditions has attracted ongoing research interest owing to their environmental friendliness and cost-effectiveness, especially compared to the traditional energy-intensive and environment-polluting Haber-Bosch process. (105) Similar to CO2RR, factors like the six-electron-transfer process, competing HER, and the unique high bonding energy of the N≡N covalent triple bond seriously hinder the FE and production rate of NRR toward NH3, making it far away from practical applications. (106,107) Notably, a record-high activity of 120.9 ugNH3 mgcat–1 h–1 is reported by Geng et al., who use MOF-derived Ru single atoms dispersed on nitrogen-doped carbon as the electrocatalyst for NRR. (108)

4. Conclusion and Outlook

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In summary, MOFs are promising precursors or sacrificial templates for preparing various advanced functional materials with desired compositions, morphologies, structures, and properties. Benefiting from many advantages including high surface area, ordered porosity, adjustable topological morphology, and diverse chemical composition of MOFs, as well as the advances in material synthesis and characterization techniques, MOF-derived functional materials have shown great opportunities for preparing advanced electrodes or high-efficiency electrocatalysts for clean, safe, and sustainable EESC systems. The uniformly distributed metal ions and organic linkers at the atomic level in MOFs provide great control on the size of active species in the derivatives. Moreover, the high specific surface area and interior spaces of derivatives facilitate the active sites exposure and mass transport, as well as accommodate the volumetric expansion during the electrochemical reaction process. Therefore, it is not surprising that the past decade has witnessed the booming development of MOF-derived electrodes or electrocatalysts with excellent performance in a wide range of EESC technologies including SCs, LIBs, SIBs, LSBs, MABs, fuel cells, water electrolysis, CO2RR, and NRR.
Nevertheless, there are still some intrinsic disadvantages of MOF-derived materials, for example, the lack of control in pore size distribution in carbonized products, and unsatisfactory catalytic stability especially in acidic medium. Therefore, more efforts are required in this ongoing field to further enhance the electrochemical performance of MOF derivatives for practical usage in future EESC devices. Several current challenges and prospective solutions are described as follows.
(1) Design and synthesize MOF-based precursors, including the novel pristine MOFs and elaborate MOF composites. The rich availability in MOFs and composites can provide more possibilities to their derivatives. Therefore, abundant fundamental knowledge about MOFs and in-depth understandings of the interfacial interactions between MOFs and the other components are essential for advanced innovations on MOF-derived functional materials. In addition, for economical consideration and future large-scale application cost-effective and scalable manufacturing of MOFs is crucial in various EESC systems.
(2) Optimize and explore postprocessing methods. Although numerous MOF-derived micro/nano-materials have been developed, their diversity in composition and structure is still insufficient. As a result, optimizing existing synthetic methods to obtain more configurations and exploring new synthetic strategies to enrich the types of derivatives are the two directions that have to be continued.
(3) Manipulate the composition, structure, and physicochemical properties of MOF-derived materials. In pursuit of this goal, the precise conversion mechanism of postprocessing and the key factors affecting the physicochemical properties of the derived materials must be thoroughly investigated. Meanwhile, it is also necessary to characterize the detailed and precise structure of derived materials by advanced technologies, such as AC-HAADF-STEM, X-ray absorption spectroscopy, and electron energy loss spectroscopy, which will help to deeply understand these mechanisms. In return, the discovery of the conversion mechanism can be a guide to optimize and explore postprocessing strategies of MOF-derived materials for enhanced performance.
(4) Optimize and improve the electrochemical performance of MOF-derived functional materials in practical EESC devices. First, the main factors that suppress the performance should be identified to establish a good understanding of the relationship among composition, structure, performance, and application. To this end, in situ or in operando structural characterizations and theoretical calculations and simulations are strongly recommended to monitor the structural evolution of the electrode/electrocatalysts during electrochemical reactions and discover the underlying reaction mechanisms. Second, efficient strategies such as surface modification, stress engineering, heterostructure, phase change, and so forth should be developed to achieve the reasonable design and control of the atomic arrangement on the surface and the electronic structure of the interface, thereby improving the catalytic performance. Last but not the least, optimization of electrode processing techniques, testing conditions, and methods is also expected to improve the final electrochemical performance in EESC devices.
(5) Develop new EESC technologies and applications of MOF-derived functional materials. Despite these challenges, the accomplishments achieved so far are indeed encouraging and the contents covered in this Mini Review are just the small tip of the iceberg for MOF-derived functional materials. With persistent research contributions and technological innovation, we should have a great chance to witness the revolution of new EESC technologies and realize more applications of MOF-derived functional materials in the fields of renewable energy and environmental science in the near future.

Author Information

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  • Corresponding Author
  • Authors
    • Xue Feng Lu - School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, SingaporeOrcidhttp://orcid.org/0000-0003-2154-2223
    • Yongjin Fang - School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, SingaporeOrcidhttp://orcid.org/0000-0002-8988-525X
    • Deyan Luan - School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, SingaporeOrcidhttp://orcid.org/0000-0003-3987-0989
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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X.W.L. acknowledges the funding support from the National Research Foundation (NRF) of Singapore via the NRF Investigatorship (NRF-NRFI2016-04).

References

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  • Abstract

    Figure 1

    Figure 1. Synthetic strategies of MOF-derived functional materials with different compositions and structures, performance improvement approaches, and their applications in various EESC systems.

    Figure 2

    Figure 2. Some typical synthesis strategies of MOF-derived functional materials for SCs. (a) Sequentially modulate the chemical reactions of ZIF-67 with water and Na2S to prepare complex CoS NBs. Reprinted with permission from ref (41). Copyright 2016, Elsevier B.V. (b) Electrospinning followed by carbonization for hollow NPs-based N-doped carbon nanofibers. Reprinted with permission from ref (42). Copyright 2017, Royal Society of Chemistry. (c) Subsequent thermal treatment toward multishelled metal oxide particles. Reprinted with permission from ref (43). Copyright 2017, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) Multistep approach to CoO/Co–Cu–S HTHSs. Reprinted with permission from ref (35). Copyright 2019, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

    Figure 3

    Figure 3. MOF-derived hollow structures for various rechargeable batteries. (a) TEM image of a triple-shelled Co3O4@Co3V2O8 NB. Reprinted with permission from ref (45). Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) TEM image and (c) discharge–charge voltage profiles at various current densities of H–Co3O4@MCNBs for lithium storage. Reprinted with permission from ref (44). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) TEM image of a Cu-CoSe2 microbox. Reprinted with permission from ref (31). Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) TEM image and (f) discharge–charge voltage profiles at various current densities of Cu-CoS2@CuxS NBs for sodium storage. Reprinted with permission from ref (32). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (g) TEM image of double-shelled CH@LDH nanocages. Reprinted with permission from ref (65). Copyright 2016, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (h) TEM image of a hollow Ni/Fe LDH polyhedron and (i) discharge–charge voltage profiles at various current densities as a sulfur host for LSBs. Reprinted with permission from ref (66). Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

    Figure 4

    Figure 4. MOF-derived atomic site electrocatalysts for alkaline ZABs and acidic PEMFCs. (a) Configuration and discharge–charge process of a typical ZAB. (b) HAADF-STEM image and corresponding EDS mapping images of Cu ISAS/NC, (c) discharge polarization and corresponding power density plots of Cu ISAS/NC based ZABs. Reprinted with permission from ref (30). Copyright 2019, Springer Nature, licensed under a Creative Commons Attribution (CC BY) license: http://creativecommons.org/licenses/by/4.0/. No changes were made. (d) HAADF-STEM image and corresponding EDS mapping images of Co1–N3PS/HC, (e) discharge polarization and corresponding power density plots of Co1–N3PS/HC based ZABs. Reprinted with permission from ref (74). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) Schematic illustration of a typical PEMFC. (g) MAADF-STEM image of 20Mn-NC-second catalyst, and (h) fuel cell performance of the best-performing 20Mn-NC-second and 20Fe-NC-second catalysts in both H2/O2 and H2/air conditions. Reprinted with permission from ref (33). Copyright 2018, Springer Nature. (i) HAADF-STEM image of Fe/Ni–Nx/OC, and (j) discharge polarization curves and the corresponding power density plots of PEMFC with Fe/Ni–Nx/OC as cathode using H2/O2 and H2/air as fuels. Reprinted with permission from ref (81). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

    Figure 5

    Figure 5. MOF-derived metal compound-based electrocatalysts for water splitting. (a) Schematic illustration, (b) TEM image, and (c) polarization curves in 0.5 M H2SO4 for HER of NFP/C hollow nanorods. Reprinted with permission from ref (34). Copyright 2019, American Association for the Advancement of Science (AAAS), distributed under a Creative Commons Attribution-NonCommercial international (CC BY-NC) license. http://creativecommons.org/licenses/by-nc/4.0/. The Authors, some rights reserved; exclusive licensee AAAS. (d) Schematic illustration, (e) TEM image, and (f) polarization curves in 1.0 M KOH for OER of Fe–Co3O4 HHNPs. Reprinted with permission from ref (83). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, licensed under a Creative Commons Attribution (CC BY) license: http://creativecommons.org/licenses/by/4.0/. We have rearranged the position of “Etching/adsorption” and moved the image representing the enlarged nanosheet from the original label location. (g) Schematic illustration, (h) AC-HAADF-STEM image, and (i) polarization curves in a broad pH range of 0–14 for OER (inset: corresponding voltages at 10 mA cm–2) of RuIrOx nanonetcages. Reprinted with permission from ref (91). Copyright 2020, Springer Nature, licensed under a Creative Commons Attribution (CC BY) license: http://creativecommons.org/licenses/by/4.0/. We have moved the “Dispersing”, “Etching”, and “Holing” from the original label locations. (j) Schematic illustration, (k) TEM image, and (l) polarization curves in 1.0 M KOH with and without 10 mM HMF in an H-type cell (inset) of MoO2–FeP@C porous nanospindles. Reprinted with permission from ref (92). Copyright 2020, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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