ACS Publications. Most Trusted. Most Cited. Most Read
Which Surface Is More Scaling Resistant? A Closer Look at Nucleation Theories for Heterogeneous Gypsum Nucleation in Aqueous Solutions

OR SEARCH CITATIONS

My Activity
Publications

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:Environ. Sci. Technol. 2022, 56, 22, 16315-16324
    Treatment and Resource Recovery

    Which Surface Is More Scaling Resistant? A Closer Look at Nucleation Theories for Heterogeneous Gypsum Nucleation in Aqueous Solutions
    Click to copy article linkArticle link copied!

    • Yiming Yin
      Yiming Yin
      Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado80523, United States
      More by Yiming Yin
    • Tianshu Li
      Tianshu Li
      Department of Civil and Environmental Engineering, George Washington University, Washington, District of Columbia20052, United States
      More by Tianshu Li
      Orcidhttps://orcid.org/0000-0002-0529-543X
    • Kuichang Zuo
      Kuichang Zuo
      The Key Laboratory of Water and Sediment Science, Ministry of Education; College of Environment Science and Engineering, Peking University, Beijing100871, China
      More by Kuichang Zuo
      Orcidhttps://orcid.org/0000-0002-3922-8702
    • Xitong Liu
      Xitong Liu
      Department of Civil and Environmental Engineering, George Washington University, Washington, District of Columbia20052, United States
      More by Xitong Liu
      Orcidhttps://orcid.org/0000-0002-5197-3422
    • Shihong Lin
      Shihong Lin
      Department of Civil and Environmental Engineering, Vanderbilt University, Nashville, Tennessee37212, United States
      More by Shihong Lin
      Orcidhttps://orcid.org/0000-0001-9832-9127
    • Yiqun Yao
      Yiqun Yao
      Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado80523, United States
      More by Yiqun Yao
    • Tiezheng Tong*
      Tiezheng Tong
      Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, Colorado80523, United States
      *Email: [email protected]. Phone: +1(970)491-1913.
      More by Tiezheng Tong
      Orcidhttps://orcid.org/0000-0002-9289-3330
    Other Access OptionsSupporting Information (1)

    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2022, 56, 22, 16315–16324
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.2c06560
    Published October 28, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

    Abstract

    Click to copy section linkSection link copied!
    Abstract Image

    Developing engineered surfaces with scaling resistance is an effective means to inhibit surface-mediated mineral scaling in various industries including desalination. However, contrasting results have been reported on the relationship between scaling potential and surface hydrophilicity. In this study, we combine a theoretical analysis with experimental investigation to clarify the effect of surface wetting property on heterogeneous gypsum (CaSO4·2H2O) formation on surfaces immersed in aqueous solutions. Theoretical prediction derived from classical nucleation theory (CNT) indicates that an increase of surface hydrophobicity reduces scaling potential, which contrasts our experimental results that more hydrophilic surfaces are less prone to gypsum scaling. We further consider the possibility of nonclassical pathway of gypsum nucleation, which proceeds by the aggregation of precursor clusters of CaSO4. Accordingly, we investigate the affinity of CaSO4 to substrate surfaces of varied wetting properties via calculating the total free energy of interaction, with the results perfectly predicting experimental observations of surface scaling propensity. This indicates that the interactions between precursor clusters of CaSO4 and substrate surfaces might play an important role in regulating heterogeneous gypsum formation. Our findings provide evidence that CNT might not be applicable to describing gypsum scaling in aqueous solutions. The fundamental insights we reveal on gypsum scaling mechanisms have the potential to guide rational design of scaling-resistant engineered surfaces.

    Copyright © 2022 American Chemical Society

    Subjects

    what are subjects

    Keywords

    what are keywords

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. Add or change your institution or let them know you’d like them to include access.

    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.2c06560.

    • Surface tension components of water, ethylene glycol, diiodomethane, and gypsum; contact angles of water, ethylene glycol, and diiodomethane on different glass substrates with varied wetting properties; surface tension components of glass substrates calculated based on the contact angle measurements of water, ethylene glycol, and diiodomethane; relationship between the surface-area-dependent term of CNT and the contact angle θN/S; relationship of the contact angle θN/S with the total surface energy and the water contact angle of the glass substrate; XPS characterization of the unmodified substrate and substrates modified with different functional silanes; measurement of gypsum solution conductivity without glass slides for 2 days; measurement of calcite solution conductivity without glass slide samples for 24 h; text for the mathematical derivation of eq 4 of the main text; and text for the calculation of interaction free energy between different substrates and water (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    Click to copy section linkSection link copied!
    Citation Statements
    Explore this article's citation statements on scite.ai
    powered by  Scite

    This article is cited by 37 publications.

    1. Marion Bellier, Mohamed E. A. Ali, Moustafa M. Abo El fadl, François Perreault. Photothermal Carbon Black Nanoparticle Coating Increases Scaling Resistance in Solar Membrane Distillation. ACS ES&T Water 2024, 4 (12) , 5925-5932. https://doi.org/10.1021/acsestwater.4c00882
    2. Ruixue Zhao, Fanxu Meng, Qinghao Wu, Zihan Zhong, Yuanfeng Liu, Ruotong Yang, Ao Li, Huan Liu, Yanyu Lu, Zishuai Zhang, Qilin Li, Huazhang Zhao, Jianfeng Li, Le Han, Kuichang Zuo. Ultra-antiwetting Membrane for Hypersaline Water Crystallization in Membrane Distillation. Environmental Science & Technology 2024, 58 (33) , 14929-14939. https://doi.org/10.1021/acs.est.4c05283
    3. Wenda Kang, Shiyu Meng, Yuchen Zhao, Jiyuan Xu, Shuai Wu, Kun Zhao, Shuo Chen, Junfeng Niu, Hongtao Yu, Xie Quan. Scaling-Free Cathodes: Enabling Electrochemical Extraction of High-Purity Nano-CaCO3 and -Mg(OH)2 in Seawater. Environmental Science & Technology 2024, 58 (31) , 14034-14041. https://doi.org/10.1021/acs.est.4c04700
    4. Ying Wang, Yaguang Zhu, Prashant Gupta, Srikanth Singamaneni, Byeongdu Lee, Young-Shin Jun. The Roles of Oil–Water Interfaces in Forming Ultrasmall CaSO4 Nanoparticles. ACS Applied Materials & Interfaces 2024, 16 (22) , 29390-29401. https://doi.org/10.1021/acsami.4c02256
    5. Tiezheng Tong, Xitong Liu, Tianshu Li, Shinyun Park, Bridget Anger. A Tale of Two Foulants: The Coupling of Organic Fouling and Mineral Scaling in Membrane Desalination. Environmental Science & Technology 2023, 57 (18) , 7129-7149. https://doi.org/10.1021/acs.est.3c00414
    6. Yan-Fang Guan, Xiang-Yu Hong, Vasiliki Karanikola, Zhangxin Wang, Weiyi Pan, Heng-An Wu, Feng-Chao Wang, Han-Qing Yu, Menachem Elimelech. Gypsum heterogenous nucleation pathways regulated by surface functional groups and hydrophobicity. Nature Communications 2025, 16 (1) https://doi.org/10.1038/s41467-025-55993-w
    7. Yuchen Geng, Jie Zhang, Jing Ren, Huifang Sun, Kuichang Zuo, Huazhang Zhao, Jianfeng Li. Hexagonal boron nitride and graphene covalent heterostructure to resist mineral scale formation and organic fouling in membrane distillation. Desalination 2025, 613 , 118999. https://doi.org/10.1016/j.desal.2025.118999
    8. Bowen Li, Pengfei Zhang, Zhan Li, Shang Xiang, Chuang Li, Aiwen Zhang, Kecheng Guan, Zhaohuan Mai, Mengyang Hu, Tomohisa Yoshioka, Hideto Matsuyama. Bioinspired hierarchical structure with intensified anti-scaling capacity for real seawater membrane distillation. Desalination 2025, 601 , 118539. https://doi.org/10.1016/j.desal.2025.118539
    9. Longfeng Hu, Zihan Liu, Jinjin Jia, Nuo Cheng, Shu Jiang, Hesong Wang, Jiaxuan Yang, Jinlong Wang, Guibai Li, Heng Liang. Antiscalant-free strategy for nanofiltration: Prolonged induction period of gypsum crystallization at ultralow pressure. Desalination 2025, 602 , 118633. https://doi.org/10.1016/j.desal.2025.118633
    10. Haiqing Chang, Zeren Ma, Huaxin Zhao, Dan Qu, Caihong Liu, Zhongsen Yan, Rui Li, Fangshu Qu, Heng Liang, Radisav D. Vidic. Regulating gypsum scaling-induced wetting in membrane distillation by heterogeneous crystallization: Role of filter media. Water Research 2025, 274 , 123146. https://doi.org/10.1016/j.watres.2025.123146
    11. Jinjin Jia, Daliang Xu, Jiaxuan Yang, Dachao Lin, Longfeng Hu, Wenxing Jin, Jinlong Wang, Weijia Gong, Guibai Li, Heng Liang. Impact of residual aluminum on nanofiltration gypsum scaling: Mitigation roles played by different species. Water Research 2025, 274 , 123106. https://doi.org/10.1016/j.watres.2025.123106
    12. Chao Wang, Yangbo Qiu, Guangzhe Wang, Long-Fei Ren, Jiahui Shao. Architecting highly hydratable and permeable dense Janus membrane for rapid and robust membrane distillation desalination. Water Research 2025, 271 , 122985. https://doi.org/10.1016/j.watres.2024.122985
    13. Jiaqi Hu, Zhangxin Wang, Tao He. Enhancing the scaling resistance of corrugated polyvinylidene fluoride hydrophobic membrane in membrane distillation: Impact of CF4 plasma modification, pulse flow, and negative pressure. Separation and Purification Technology 2025, 354 , 128704. https://doi.org/10.1016/j.seppur.2024.128704
    14. Tiezheng Tong, Shinyun Park, Yiqun Yao. A tale of two minerals: contrasting behaviors and mitigation strategies of gypsum scaling and silica scaling in membrane desalination. Frontiers of Environmental Science & Engineering 2025, 19 (1) https://doi.org/10.1007/s11783-025-1923-9
    15. Yingyuan Zhu, Fangshu Qu, Dan Qu, Zhongsen Yan, Bin Liu, Caihong Liu, Haiqing Chang, Heng Liang, Radisav D. Vidic. In-line granular filtration for mitigating gypsum scaling in membrane distillation. Journal of Membrane Science 2025, 713 , 123259. https://doi.org/10.1016/j.memsci.2024.123259
    16. Jinjin Jia, Jinlong Wang, Dachao Lin, Jing Zhao, Hesong Wang, Longfeng Hu, Jiaxuan Yang, Han Zhang, Guibai Li, Heng Liang. Impacts of distinct residual aluminum on gypsum scaling in nanofiltration: Identification of key species. Desalination 2024, 591 , 118057. https://doi.org/10.1016/j.desal.2024.118057
    17. Chao Wang, Yangbo Qiu, Chenglin Zhang, Feng Li, Long-Fei Ren, Jiahui Shao. Developing high-flux dense Janus membrane with robust wetting and scaling resistance: A systematic comparison with Omniphobic membranes. Desalination 2024, 591 , 118060. https://doi.org/10.1016/j.desal.2024.118060
    18. Chao Wang, Yangbo Qiu, Chengyi Wang, Long-Fei Ren, Jiahui Shao. Insights into gypsum and silica scaling behaviors of dense Janus membranes in membrane distillation: The effect of varied surface properties. Desalination 2024, 592 , 118147. https://doi.org/10.1016/j.desal.2024.118147
    19. Jung Bin Yang, Jaehyeon Jeon, Jae Woo Sim, Jaehee Cho, Hanmin Jang, Dong Rip Kim. Anti-fouling characteristics of super-wicking surfaces inspired by cornea. International Communications in Heat and Mass Transfer 2024, 159 , 108157. https://doi.org/10.1016/j.icheatmasstransfer.2024.108157
    20. Ye Qiu, Tong Zhang, Ping Zhang. Micro/nano plastics inhibit the formation of barium sulfate scale on metal surface. Journal of Hazardous Materials 2024, 480 , 136151. https://doi.org/10.1016/j.jhazmat.2024.136151
    21. Meng Wang, Wangzhe Sun, Dongshuai Hou, Muhan Wang, Heping Zheng, Jun Zhang, Binmeng Chen. Stepwise modeling approach to explore the interfacial behavior of Ca(OH)2/Sulfate. Journal of Building Engineering 2024, 98 , 111005. https://doi.org/10.1016/j.jobe.2024.111005
    22. Mariana Hernandez Molina, Yusi Li, W. Shane Walker, Rafael Verduzco, Mary Laura Lind, François Perreault. Desalination of complex saline waters: sulfonated pentablock copolymer pervaporation membranes do not fail when exposed to scalants and surfactants. Journal of Membrane Science Letters 2024, 4 (2) , 100080. https://doi.org/10.1016/j.memlet.2024.100080
    23. Rui Zhang, Yunhuan Chen, Hailong Wang, Xiaoxiao Duan, Yongsheng Ren. A Janus membrane with silica nanoparticles interlayer for treating coal mine water via membrane distillation. Separation and Purification Technology 2024, 350 , 127995. https://doi.org/10.1016/j.seppur.2024.127995
    24. Afsana Munni, Mohammed A. Bashammakh, Marion Bellier, Ali Ansari, Mohamed E. A. Ali, H. Enis Karahan, Rafiqul Islam, Treavor H. Boyer, François Perreault. Surface characteristics of thin film composite polyamide membranes dictate silver nanoparticle loading efficacy. RSC Applied Interfaces 2024, 1 (6) , 1186-1197. https://doi.org/10.1039/D4LF00088A
    25. Meng Wang, Xiaobing Zuo, Raynara M.S. Jacovone, Ryan O'Hara, Abhishek Narayan Mondal, Ayse Asatekin, Debora F. Rodrigues. Influence of zwitterionic amphiphilic copolymers on heterogeneous gypsum formation: A promising approach for scaling resistance. Water Research 2024, 266 , 122439. https://doi.org/10.1016/j.watres.2024.122439
    26. Guangli Ye, Kun Yu, Mengyuan Niu, Qian Wang, Menghan Yu, Xiongbo Dong, Huaming Yang. Facet engineering of minerals for effective oil-water separation. Chemical Engineering Journal 2024, 487 , 150556. https://doi.org/10.1016/j.cej.2024.150556
    27. Mohamed E.A. Ali, Afsana Munni, Mohammed A. Bashammakh, François Perreault. Spray-coated porous photothermal layer on PTFE membranes for robust anti-scaling and solar membrane distillation. Desalination 2024, 573 , 117196. https://doi.org/10.1016/j.desal.2023.117196
    28. Hongting Wan, Fanxi Zeng, Huarong Yu, Zhouyang Zhuang, Alicia Kyoungjin An, Senlin Shao, Fangshu Qu. Crossflow-induced membrane vibration and its effects on fouling and scaling in direct contact membrane distillation. Journal of Membrane Science 2024, 694 , 122410. https://doi.org/10.1016/j.memsci.2024.122410
    29. R. Jiménez-Robles, V. Martínez-Soria, M. Izquierdo, Lo-I. Chen, K. Le Corre Pidou, E.J. McAdam. Membrane-assisted reactive crystallisation for the recovery of dissolved phosphorus in vivianite form from liquid effluents. Separation and Purification Technology 2023, 326 , 124712. https://doi.org/10.1016/j.seppur.2023.124712
    30. Haiqing Chang, Yingyuan Zhu, Lin Huang, Zhongsen Yan, Fangshu Qu, Heng Liang. Mineral scaling induced membrane wetting in membrane distillation for water treatment: Fundamental mechanism and mitigation strategies. Water Research 2023, 247 , 120807. https://doi.org/10.1016/j.watres.2023.120807
    31. Zhan Li, Pengfei Zhang, Yu-Hsuan Chiao, Kecheng Guan, Ralph Rolly Gonzales, Ping Xu, Zhaohuan Mai, Guorong Xu, Mengyang Hu, Tooru Kitagawa, Tomohisa Yoshioka, Hideto Matsuyama. Improvement of anti-wetting and anti-scaling properties in membrane distillation process by a facile fluorine coating method. Desalination 2023, 566 , 116936. https://doi.org/10.1016/j.desal.2023.116936
    32. Niklas Wehmann, Christoph Lenting, Sandro Jahn. Calcium sulfates in planetary surface environments. Global and Planetary Change 2023, 230 , 104257. https://doi.org/10.1016/j.gloplacha.2023.104257
    33. Chunyi Sun, Bin Lin, Xiangyong Zheng, Yingchao Dong, Min Zhao, Chuyang Y. Tang. Robust ceramic-based graphene membrane for challenging water treatment with enhanced fouling and scaling resistance. Water Research 2023, 243 , 120348. https://doi.org/10.1016/j.watres.2023.120348
    34. Honglong Zhang, Xuan Zhao. Enhanced Anti‐Wetting Methods of Hydrophobic Membrane for Membrane Distillation. Advanced Science 2023, 10 (23) https://doi.org/10.1002/advs.202300598
    35. Chao Wang, Zhongbao Ma, Yangbo Qiu, Chengyi Wang, Long-Fei Ren, Jiangnan Shen, Jiahui Shao. Patterned dense Janus membranes with simultaneously robust fouling, wetting and scaling resistance for membrane distillation. Water Research 2023, 242 , 120308. https://doi.org/10.1016/j.watres.2023.120308
    36. Yewei Wang, Jie Liu, Zhuo Li, Xin Liu, Weiyi Li. Revisiting scaling of calcium sulfate in membrane distillation: Uncertainty of crystal-membrane interactions. Water Research 2023, 239 , 120060. https://doi.org/10.1016/j.watres.2023.120060
    37. Mohamed E.A. Ali, Rayan Alghanayem, Aislinn Varela, Marion Bellier, François Perreault. Scaling mitigation in direct contact membrane distillation using air microbubbles. Desalination 2023, 549 , 116348. https://doi.org/10.1016/j.desal.2022.116348
    Download PDF
    Go to Environmental Science & Technology
    Get e-Alerts
    Get e-Alerts

    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2022, 56, 22, 16315–16324
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.2c06560
    Published October 28, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

    Article Views

    2275

    Altmetric

    -

    Citations

    37
    Learn about these metrics

    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.