Conflicting Roles of Coordination Number on Catalytic Performance of Single-Atom Pt CatalystsClick to copy article linkArticle link copied!
- Dahong HuangDahong HuangSchool of Environment and Civil Engineering, Dongguan University of Technology, Dongguan, Guangdong 523808, P.R. ChinaDepartment of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United StatesMore by Dahong Huang
- Ning HeNing HeSchool of Chemical Engineering, Dalian University of Technology, Dalian 116024, P.R. ChinaMore by Ning He
- Qianhong ZhuQianhong ZhuDepartment of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United StatesMore by Qianhong Zhu
- Chiheng ChuChiheng ChuDepartment of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United StatesMore by Chiheng Chu
- Seunghyun WeonSeunghyun WeonSchool of Health and Environmental Science, Korea University, Seoul 02841, KoreaMore by Seunghyun Weon
- Kali RigbyKali RigbyDepartment of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United StatesMore by Kali Rigby
- Xuechen ZhouXuechen ZhouDepartment of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United StatesMore by Xuechen Zhou
- Lei XuLei XuSchool of Environment and Civil Engineering, Dongguan University of Technology, Dongguan, Guangdong 523808, P.R. ChinaMore by Lei Xu
- Junfeng Niu*Junfeng Niu*Email: [email protected]. Tel/Fax: +86-769-22863180.School of Environment and Civil Engineering, Dongguan University of Technology, Dongguan, Guangdong 523808, P.R. ChinaMore by Junfeng Niu
- Eli StavitskiEli StavitskiNational Synchrotron Light Source- II, Brookhaven National Laboratory, Upton, New York 11973, United StatesMore by Eli Stavitski
- Jae-Hong Kim*Jae-Hong Kim*Email: [email protected]. Tel.: +1-203-432-4386. Fax: +1-203-432-4387.Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520, United StatesMore by Jae-Hong Kim
Abstract
Tailoring the coordination number (CN) of metal atoms has been increasingly recognized as one of the strategies to enhance the catalytic performance of single-atom catalysts (SACs). We here present the single-atom Pt loaded onto a semiconductor SiC substrate (Pt1/SiC) with a high loading of up to 9.6 wt % and a precise control of its CN from 3 to 5. The CN tuning was enabled by binding organic linkers on the substrate surface and retaining the metal-linker bonds after photoreduction and mild thermal treatment from 80 to 160 °C. At a higher temperature, Pt became coordinated with additional oxygen atoms from the surface Si–OH groups and organic linkers. This resulted in the increase of the CN from 3 for Pt1 treated at 80 °C to 5 at 160 °C. The Pt1/SiCs with varying CNs effectively broke C–Br bonds in the model brominated compounds through both thermocatalysis using H2 and photocatalysis using H+ as the source for strongly reducing atomic hydrogen (Hatom). The thermocatalytic debromination kinetics increased with the decreasing CN. However, photocatalytic debromination kinetics were independent of the CN, contradictory to the prevalent understanding in literature. We attribute the differential CN effects on these two catalytic schemes to the differences in the pathways for the formation of Hatom as well as the rate-limiting step of the overall reaction pathways. Our study presents a unique and important example as to how the performance of SACs and the role of CN can significantly vary depending on the catalytic schemes.
Cited By
This article is cited by 28 publications.
- Honghui Gong, Longxing Wei, Qi Li, Juan Zhang, Fei Wang, Jing Ren, Xian-Lei Shi. Electron-Rich Ru Supported on N-Doped Coffee Biochar for Selective Reductive Amination of Furfural to Furfurylamine. Langmuir 2024, 40
(17)
, 8950-8960. https://doi.org/10.1021/acs.langmuir.4c00112
- Wei Ran, Huachao Zhao, Xiaoling Zhang, Shiwei Li, Jie-Fang Sun, Jingfu Liu, Rui Liu, Guibin Jiang. Critical Review of Pd-Catalyzed Reduction Process for Treatment of Waterborne Pollutants. Environmental Science & Technology 2024, 58
(7)
, 3079-3097. https://doi.org/10.1021/acs.est.3c09198
- Bingxin Dou, Guanlong Wang, Xiaoli Dong, Xiufang Zhang. Improved H2O2 Electrosynthesis on S-doped Co–N–C through Cooperation of Co–S and Thiophene S. ACS Applied Materials & Interfaces 2024, 16
(6)
, 7374-7383. https://doi.org/10.1021/acsami.3c18879
- Jinwook Lee, Jooyoun Kim. Cooperative Design of the Ag3PO4/NH2-MIL-88B (Fe/Co) Heterojunction Integrated with Conductive Polypyrrole for Advanced Photocatalytic Water Purification. ACS Omega 2024, 9
(5)
, 5942-5953. https://doi.org/10.1021/acsomega.3c09625
- Liangzhong Li, Chenyu Yang, Yile Yan, Xian Xiao, Yang Yu, Chang Liu, Ruixue Ma, Lun Lu, Xiaoyun Fan, Da Chen, Yabing Meng, Long Yan, Yunjiang Yu. Engineering Hexacoordination-Structured Co Single-Atom Sites (Co–N4+2) to Boost Peroxydisulfate Activation in Advanced Oxidation Processes. ACS ES&T Engineering 2023, 3
(11)
, 1908-1917. https://doi.org/10.1021/acsestengg.3c00262
- Kali Rigby, Dahong Huang, Denis Leshchev, Hyun Jeong Lim, Hyeyeon Choi, Aidan Francis Meese, Seunghyun Weon, Eli Stavitski, Jae-Hong Kim. Palladium Single-Atom (In)Stability Under Aqueous Reductive Conditions. Environmental Science & Technology 2023, 57
(36)
, 13681-13690. https://doi.org/10.1021/acs.est.3c03346
- Jing Wang, Yongbing Xie, Guangfei Yu, Lichang Yin, Jiadong Xiao, Yuxian Wang, Weiguang Lv, Zhi Sun, Jae-Hong Kim, Hongbin Cao. Manipulating Selectivity of Hydroxyl Radical Generation by Single-Atom Catalysts in Catalytic Ozonation: Surface or Solution. Environmental Science & Technology 2022, 56
(24)
, 17753-17762. https://doi.org/10.1021/acs.est.2c06836
- Xuanhao Wu, Jae-Hong Kim. Outlook on Single Atom Catalysts for Persulfate-Based Advanced Oxidation. ACS ES&T Engineering 2022, 2
(10)
, 1776-1796. https://doi.org/10.1021/acsestengg.2c00187
- Baljeet Singh, Manoj B. Gawande, Arun D. Kute, Rajender S. Varma, Paolo Fornasiero, Peter McNeice, Rajenahally V. Jagadeesh, Matthias Beller, Radek Zbořil. Single-Atom (Iron-Based) Catalysts: Synthesis and Applications. Chemical Reviews 2021, 121
(21)
, 13620-13697. https://doi.org/10.1021/acs.chemrev.1c00158
- Dahong Huang, David J. Kim, Kali Rigby, Xuechen Zhou, Xuanhao Wu, Aidan Meese, Junfeng Niu, Eli Stavitski, Jae-Hong Kim. Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination. Environmental Science & Technology 2021, 55
(19)
, 13306-13316. https://doi.org/10.1021/acs.est.1c04294
- Hanyu Hu, Yanyan Zhao, Yue Zhang, Jiangbo Xi, Jian Xiao, Sufeng Cao. Performance Regulation of Single-Atom Catalyst by Modulating the Microenvironment of Metal Sites. Topics in Current Chemistry 2023, 381
(5)
https://doi.org/10.1007/s41061-023-00434-9
- Zhongsen Wang, Ming Cheng, Yi Liu, Zewei Wu, Huayu Gu, Yi Huang, Lizhi Zhang, Xiao Liu. Dual‐Atomic‐Site Catalysts for Molecular Oxygen Activation in Heterogeneous Thermo‐/Electro‐catalysis. Angewandte Chemie 2023, 135
(22)
https://doi.org/10.1002/ange.202301483
- Zhongsen Wang, Ming Cheng, Yi Liu, Zewei Wu, Huayu Gu, Yi Huang, Lizhi Zhang, Xiao Liu. Dual‐Atomic‐Site Catalysts for Molecular Oxygen Activation in Heterogeneous Thermo‐/Electro‐catalysis. Angewandte Chemie International Edition 2023, 62
(22)
https://doi.org/10.1002/anie.202301483
- Dan Sun, Yajie Chen, Xinyan Yu, Yuejia Yin, Guohui Tian. Engineering high-coordinated cerium single-atom sites on carbon nitride nanosheets for efficient photocatalytic amine oxidation and water splitting into hydrogen. Chemical Engineering Journal 2023, 462 , 142084. https://doi.org/10.1016/j.cej.2023.142084
- Haiyan An, Liangliang Liu, Nan Song, Hongmei Zhu, Yu Tang. Rational design and synthesis of cerium dioxide-based nanocomposites. Nano Research 2023, 16
(3)
, 3622-3640. https://doi.org/10.1007/s12274-022-4941-y
- Joshua Meléndez-Rivera, Juan A. Santana. Density Functional Calculations of the Sequential Adsorption of Hydrogen on Single Atom and Small Clusters of Pd and Pt Supported on Au(111). Electrocatalysis 2023, 14
(2)
, 325-331. https://doi.org/10.1007/s12678-022-00802-x
- Shang Li, Yuxing Xu, Hengwei Wang, Botao Teng, Qin Liu, Qiuhua Li, Lulu Xu, Xinyu Liu, Junling Lu. Tuning the CO
2
Hydrogenation Selectivity of Rhodium Single‐Atom Catalysts on Zirconium Dioxide with Alkali Ions. Angewandte Chemie 2023, 135
(8)
https://doi.org/10.1002/ange.202218167
- Shang Li, Yuxing Xu, Hengwei Wang, Botao Teng, Qin Liu, Qiuhua Li, Lulu Xu, Xinyu Liu, Junling Lu. Tuning the CO
2
Hydrogenation Selectivity of Rhodium Single‐Atom Catalysts on Zirconium Dioxide with Alkali Ions. Angewandte Chemie International Edition 2023, 62
(8)
https://doi.org/10.1002/anie.202218167
- Xueshan Hu, Daxian Zuo, Shaoru Cheng, Sihui Chen, Yang Liu, Wenzhong Bao, Sili Deng, Stephen J. Harris, Jiayu Wan. Ultrafast materials synthesis and manufacturing techniques for emerging energy and environmental applications. Chemical Society Reviews 2023, 52
(3)
, 1103-1128. https://doi.org/10.1039/D2CS00322H
- Chong Wang, Chen Guo. Nitrogen atom coordination tuned transition metal catalysts for NO oxidation and reduction. Chemosphere 2022, 309 , 136735. https://doi.org/10.1016/j.chemosphere.2022.136735
- Wei Tan, Shaohua Xie, Duy Le, Weijian Diao, Meiyu Wang, Ke-Bin Low, Dave Austin, Sampyo Hong, Fei Gao, Lin Dong, Lu Ma, Steven N. Ehrlich, Talat S. Rahman, Fudong Liu. Fine-tuned local coordination environment of Pt single atoms on ceria controls catalytic reactivity. Nature Communications 2022, 13
(1)
https://doi.org/10.1038/s41467-022-34797-2
- Bin Han, Yu Luo, Yuanfang Lin, Bo Weng, Dehua Xia, Yang Zhou, Chaoting Guan, Zhen Wang, Xipeng Wei, Jin Jiang. Microenvironment engineering of single-atom catalysts for persulfate-based advanced oxidation processes. Chemical Engineering Journal 2022, 447 , 137551. https://doi.org/10.1016/j.cej.2022.137551
- Weiqiong Zheng, Ran Zhu, Huijuan Wu, Tian Ma, Hongju Zhou, Mi Zhou, Chao He, Xikui Liu, Shuang Li, Chong Cheng. Tailoring Bond Microenvironments and Reaction Pathways of Single‐Atom Catalysts for Efficient Water Electrolysis. Angewandte Chemie 2022, 134
(41)
https://doi.org/10.1002/ange.202208667
- Weiqiong Zheng, Ran Zhu, Huijuan Wu, Tian Ma, Hongju Zhou, Mi Zhou, Chao He, Xikui Liu, Shuang Li, Chong Cheng. Tailoring Bond Microenvironments and Reaction Pathways of Single‐Atom Catalysts for Efficient Water Electrolysis. Angewandte Chemie International Edition 2022, 61
(41)
https://doi.org/10.1002/anie.202208667
- Wenjing Xu, Hao Tang, Hongfei Gu, Hongyan Xi, Pengfei Wu, Benliang Liang, Qingqing Liu, Wenxing Chen. Research progress of asymmetrically coordinated single-atom catalysts for electrocatalytic reactions. Journal of Materials Chemistry A 2022, 10
(28)
, 14732-14746. https://doi.org/10.1039/D2TA03034A
- Shangchun Lv, Mengxi Pei, Yuxiang Liu, Zhichun Si, Xiaodong Wu, Rui Ran, Duan Weng, Feiyu Kang. An isolation strategy to anchor atomic Ni or Co cocatalysts on TiO2(A) for photocatalytic hydrogen production. Nano Research 2022, 15
(7)
, 5848-5856. https://doi.org/10.1007/s12274-022-4217-6
- Zhun Zhang, Hengyu Li, Danfeng Wu, Lina Zhang, Jiwei Li, Junli Xu, Sen Lin, Abhaya K. Datye, Haifeng Xiong. Coordination structure at work: Atomically dispersed heterogeneous catalysts. Coordination Chemistry Reviews 2022, 460 , 214469. https://doi.org/10.1016/j.ccr.2022.214469
- Baisong Chang, Liqin Zhang, Shaolong Wu, Ziyan Sun, Zhen Cheng. Engineering single-atom catalysts toward biomedical applications. Chemical Society Reviews 2022, 51
(9)
, 3688-3734. https://doi.org/10.1039/D1CS00421B
Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.
Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.
The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.