电催化合成过氧化氢用于环境消毒

doi:10.1016/S1872-2067(20)63781-0

催化学报 ›› 2021, Vol. 42 ›› Issue (12): 2149-2163.DOI: 10.1016/S1872-2067(20)63781-0

电催化合成过氧化氢用于环境消毒

曾亚超, 武刚^*()

纽约州立大学布法罗分校化学与生物工程系, 纽约州布法罗14260, 美国

收稿日期:2021-01-06 接受日期:2021-01-06 出版日期:2021-12-18 发布日期:2021-05-06
通讯作者: 武刚

Electrocatalytic H₂O₂ generation for disinfection

Yachao Zeng, Gang Wu^*()

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United States

Received:2021-01-06 Accepted:2021-01-06 Online:2021-12-18 Published:2021-05-06
Contact: Gang Wu
About author:* Tel: +1-716-6458618; Fax: +1-716-6453822; E-mail: gangwu@buffalo.edu
Gang Wu is a professor in the Department of Chemical and Biological Engineering at the University at Buffalo, the State University of New York (SUNY). He obtained all of his B.S., M.S. and Ph.D. degrees at the Harbin Institute of Technology in 1997, 1999, and 2004, respectively. He performed extensive postdoctoral training at Tsinghua University (2004‒2006), the University of South Carolina (2006‒2008), and Los Alamos National Laboratory (LANL, 2008‒2010). Then he was promoted to a staff scientist at LANL (2010‒2014). He joined the University of Buffalo in 2014 as a tenure-track assistant professor and was quickly promoted to a tenured associate professor in 2018 and a full professor in 2020. His research focuses on functional materials and catalysts for electrochemical energy storage and conversion. He has published more than 250 papers, which have been cited more than > 27,000 times with an H index of 82 (Google Scholar) by Feb 2021. Clarivate Analytics (Web of Science) continuously acknowledged Dr. Wu as one of the Highly Cited Researchers in 2018, 2019, and 2020. He served as the Editorial Board of Chinese Journal of Catalysis since 2020.

摘要/Abstract

摘要：

流行性疾病贯穿整个人类历史, 伴随全球人口流动, 它们可能演变成大型流行病. 时至今日, 我们仍在见证已知和新生的病原体对人类历史格局的改变. 在与流行性疾病的抗争中, 诸如紫外线辐射、巴氏杀菌和化学氧化法等技术被用于病原体的消杀和抗体的研制. 然而, 这些技术在环境消毒方面存在诸多不利, 譬如过长的消杀时间、昂贵的特殊设备以及伴生的环境污染.

过氧化氢是一种环境友好的多功能氧化剂, 其分解的最终产物是氧气和水, 广泛用于伤口消毒、纸浆和纺织品漂白、废水废气处理、化学合成、半导体清洗以及洗涤剂. 目前, 过氧化氢的生产严重依赖于传统的蒽醌法, 该技术由Riedl和Pfleiderer于1939年提出, 并沿用至今. 然而, 蒽醌法能耗高, 该技术仅在较大规模上经济可行. 不稳定的过氧化氢溶液存在危险性, 这对大宗过氧化氢的运输和存储提出了额外的挑战.

电化学合成过氧化氢被认为可有效替代传统蒽醌法, 其反应条件温和, 所需反应物是环境中广泛存在的水和氧气; 与可再生能源相结合, 有望实现分布式原位生产过氧化氢. 过氧化氢既可以通过两电子的水氧化反应生成, 又可以经由两电子的氧还原反应产生. Berl等在上世纪30年代首次报道了经由两电子的氧还原反应合成过氧化氢, 并随后在1991年将其商业化(亦即Huron-Dow法). 自此, Huron-Dow法被广泛用于纸浆和纸张的漂白过程. 最近, Huron-Dow法进一步演变为电子-芬顿工艺, 并被广泛用于饮用水净化和污水处理. 目前, 涉及高活性和高选择性的电化学合成过氧化氢的优秀综述见诸各大期刊; 但是鲜有综述探讨该技术在环境消毒方面的应用.

为了探寻提升公共卫生安全的有效替代方法, 本文探讨了在电催化制备过氧化氢在环境消毒方面的可行性. 本文涵盖三个主题, 从基础理论到实践两个层次探讨了该技术在实际应用中的可行性. 首先, 回顾了H₂O₂消杀病原体的机理; 其次, 讨论了影响电催化制备过氧化氢的关键因素, 并对现有的用于两电子水氧化和氧还原的催化剂进行了系统性的评述; 最后, 讨论了电极和电解池的合理设计, 以实现电催化制备过氧化氢在实际中的应用. 本文试图为最终实现电催化制备过氧化氢在环境消毒, 尤其是公共卫生领域, 提供可寻的研究方向.

关键词: 过氧化氢, 氧还原, 环境消毒, 电化学合成, 金属单原子催化剂

Abstract:

Epidemics are threatening public health and social development. Emerging as a green disinfectant, H₂O₂ can prevent the breakout of epidemics in migration. Electrochemical H₂O₂ production powered by renewable electricity provides a clean and decentralized solution for on-site disinfection. This review firstly discussed the efficacy of H₂O₂ in disinfection. Then necessary fundamental principles are summarized to gain insight into electrochemical H₂O₂ production. The focus is on exploring pathways to realize a highly efficient H₂O₂ production. Progress in advanced electrocatalysts, typically single-atom catalysts for the two-electron oxygen reduction reaction (2e^- ORR), are highlighted to provide high H₂O₂ selectivity design strategies. Finally, a rational design of electrode and electrolytic cells is outlined to realize the on-site disinfection. Overall, this critical review contributes to exploiting the potentials and constraints of electrochemical H₂O₂ generation in disinfection and pinpoints future research directions required for implementation.

Key words: Hydrogen peroxide, Oxygen reduction, Disinfection, Electrosynthesis, Single metal atom catalysts

曾亚超, 武刚. 电催化合成过氧化氢用于环境消毒[J]. 催化学报, 2021, 42(12): 2149-2163.

Yachao Zeng, Gang Wu. Electrocatalytic H₂O₂ generation for disinfection[J]. Chinese Journal of Catalysis, 2021, 42(12): 2149-2163.

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图/表 9

Fig. 1. Destruction of infectious agents by ROS. The susceptibility to oxidative damages can be ordered as viruses > prions > Gram (-) bacteria > Gram (+) bacteria > yeasts > molds. ROS will eventually oxidize organic matter and dead microbial cells into CO2 and H2O. Reproduced with permission [35]. Copyright 2015, Springer.

Fig. 2. Fe(III) catalyzed Haber-Weiss Cycle/Fenton reaction.

Fig. 3. Electrochemical H2O2 generation via the ORR, the WOR and the association pathways with the transient intermediates on the different catalyst surfaces.

Fig. 4. (a) A schematic illustrating the possible reaction pathway steered by local concentrate O2. (b) Optical image for PTFE-patterned glassy carbon (GC) at 2.05 VRHE in 1.0 M Na2CO3 electrolyte. (c) Adhesive force measurements of O2 gas bubble on pristine GC, 300-GC and 200-GC electrodes, demonstrating enhanced O2 adhesive force of the GC surface by PTFE coating. (d) Comparison of total current densities in the pristine carbon fiber paper (CFP), CFP-5%, CFP-20% and CFP-60% catalysts. (e) The FE of pristine GC, 300-GC and 200-GC catalysts at 2.05 VRHE in 1.0 M Na2CO3 electrolyte. (f) A comparison of H2O2 generation rates of CFP-60% catalyst against other catalyst systems under different applied potentials. Reproduced with permission [92]. Copyright 2020, Springer Nature.

Fig. 5. (a) A general synthetic strategy for platinoid SACs; HAADF-STEM image (b) and Pt L3-edge k3-weighted EXAFS spectrum and the best fit (c) for 3Pt/CNT_IL_SiO2; (d) ORR activity and selectivity of 3Pt/CNT_IL_SiO2 in 0.1 M HClO4; (e) A comparison of H2O2 yields in nanoparticle and single atom catalysts at -0.5 mA cm-2, in which M/CNT and M/CNT_IL_SiO2 are denoted as MNP and M1, respectively; (f) Linear relationship between the DFT-calculated ΔGO values and the experimentally determined H2O2 yields of the SACs; (g) Volcano plot between the O binding energies and the onset potentials for the 2e- ORR pathway for SACs and NP catalysts. Reproduced with permission [127]. Copyright 2020, American Society of Chemistry.

Fig. 6. (a) Schematic illustration of various M-N-C SACs (M = Mn, Fe, Co, Ni, Cu) and their preferred ORR pathways. (b) Correlation of binding energy of *OOH, *O, and *OH on M-SAC (M = Mn, Fe, Co, Ni, and Cu) and d-bond center (open circle) of M atom in M-SAC (M = Mn, Fe, Co, Ni, and Cu). Reprinted with permission [118]. Copyright 2020, Elsevier Inc. (c) H2O2 production current as a function of the binding energy of OH* intermediate. (d) H2O2 selectivity (H2O2 %) and the electrons transfer number (n) at 0.1 VRHE over various M-N-C SACs. Reproduced with permission [119]. Copyright 2019, American Society of Chemistry. Comparison of H2O2 selectivity (e) and H2O2 current at 0.7 V (f) for NG(O), Co1-NG(O) and Co1-NG(R). (g) ORR volcano plots for the production of H2O (blue) and H2O2 (red). Red and blue data points are Co-N4/graphene catalyst with electron-rich species (O*/2O*) and electron-poor species (4H*/2H*) adsorbed close to the cobalt atom, respectively. Reproduced with permission [128]. Copyright 2020 Springer Nature.

Fig. 7. (a) Reconstructed atom probe tomography of Fe-CNT catalyst. TEM (b), HAADF-STEM (c) and XAS (d) characterizations of Fe-CNT catalyst. (e) Overall ORR current and (f) corresponding H2O2 selectivity of Fe-, Pd-, Co-, Mn-CNT catalysts. (g) Schematic illustration of electrochemical H2O2 generation for water disinfection, powering with renewable energy. (h) The disinfection efficacy as a function of reaction time. Reprinted with permission from Ref. [117]. Copyright 2019, Nature Publishing Group.

Fig. 8. (a) Schematic illustrations of the NADE fabrication process and the three-phase electrocatalytic system; In-panel (b) and cross-sectional (c) SEM images of modified carbon felt with contact angle (inset); (d) The concentration profiles of H2O2 production in different systems at 60 mA cm-2 current density. Reproduced with permission [147]. Copyright 2020, Springer Nature.

Fig. 9. (a) Schematic diagram of the H2O2 generation in a membrane-free electrolyzer mode. Reprinted with permission [153]. Copyright 2017, The Royal Society of Chemistry. (b) Membrane-based flow reactor containing a MEA. The MEA is sandwiched between the anode and cathode current collectors with flow field patterns. Reprinted with permission [27]. Copyright 2020, American Society of Chemistry. (c) Electrochemical H2O2 generation by using pure H2 and O2 streams separately introduced to the anode and cathode. SE denotes a solid electrolyte, which consisted of either functionalized styrene-divinylbenzene copolymer microspheres or inorganic CsxH3?xPW12O40 in this study. Electrochemically produced H+ and HO2-, driven by the electric field, cross in the porous SE layer and form H2O2. H2O2 with no impurities is carried out by flowing DI water through the porous SE layer. Reprinted with permission [154]. Copyright 2019, AAAS. (d) Illustration of overall phase-transfer strategy for electrochemical H2O2 generation. Reproduced with permission [155]. Copyright 2019, Elsevier Inc.

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电催化合成过氧化氢用于环境消毒

Electrocatalytic H₂O₂ generation for disinfection

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电催化合成过氧化氢用于环境消毒

Electrocatalytic H2O2 generation for disinfection

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Electrocatalytic H₂O₂ generation for disinfection