分子催化剂催化水氧化过程及其O-O成键机理

doi:10.1016/S1872-2067(20)63681-6

催化学报 ›› 2021, Vol. 42 ›› Issue (8): 1253-1268.DOI: 10.1016/S1872-2067(20)63681-6

分子催化剂催化水氧化过程及其O-O成键机理

张学鹏, 王红艳, 郑浩铨, 张伟, 曹睿^*()

陕西师范大学化学化工学院, 应用表面与胶体化学教育部重点实验室, 陕西西安710119

收稿日期:2020-08-11 接受日期:2020-09-22 出版日期:2021-08-18 发布日期:2020-12-10
通讯作者: 曹睿
作者简介:^*, 电子信箱: ruicao@snnu.edu.cn
基金资助:
国家自然科学基金(21101170);国家自然科学基金(21573139);国家自然科学基金(21773146);霍英东青年教师基金;中央高校基本科研基金;陕西师范大学研究经费

O-O bond formation mechanisms during the oxygen evolution reaction over synthetic molecular catalysts

Xue-Peng Zhang, Hong-Yan Wang, Haoquan Zheng, Wei Zhang, Rui Cao^*()

Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an 710119, Shaanxi, China

Received:2020-08-11 Accepted:2020-09-22 Online:2021-08-18 Published:2020-12-10
Contact: Rui Cao
About author:^*, E-mail: ruicao@snnu.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China(21101170);This work was supported by the National Natural Science Foundation of China(21573139);This work was supported by the National Natural Science Foundation of China(21773146);Fok Ying-Tong Education Foundation for Outstanding Young Teachers in University (by the Ministry of Education of China);Fundamental Research Funds for the Central Universities;the Research Funds of Shaanxi Normal University

摘要/Abstract

摘要：

随着化石燃料的不断消耗和生存环境的日益恶化, 可再生、清洁且环境友好的新能源逐渐受到广泛关注与利用. 太阳能作为一种洁净的可再生能源, 在自然界中, 植物可以通过光合作用将太阳能转换成化学能. 在该过程中, 水分子在光系统II中被氧化而释放出氧气, 伴随生成的质子和电子进一步将二氧化碳转化为蕴含生物质能的碳水化合物.
在光系统II中, 叶绿素P680被光照激发生成阳离子自由基P680 ^•+, 其具有很强的氧化能力, 可以从附近的析氧中心中夺取电子. 析氧中心通过这一过程失去4个电子, 可以将两分子水氧化生成一分子氧气和4个质子. 作为水裂解的半反应之一, 水氧化在热力学方面需要很多能量来断裂4个O-H键(ΔE = 1.23 V vs. NHE), 在动力学方面涉及4个氢原子与2个氧原子的重组以及氧气的释放, 因而水氧化析氧是一个非常缓慢的过程, 如何高效稳定地催化水氧化一直是人们研究的热点和难点. 研究发现, 自然界中存在的析氧中心为Mn₄CaO_x的钙锰簇合物, 在水氧化过程中生成的Mn=O物种可以被游离的水分子亲核进攻形成O-O键, 也可以与桥连μ-O(H)反应生成O-O键. 通过对析氧中心持续的研究, 在过去几十年中设计合成了一系列具有水氧化催化活性的基于金属配合物的分子催化剂.
分子催化剂催化水氧化一般主要分为金属-氧物种的演化过程以及O-O成键过程. 通常, 金属-氧物种可以通过失电子或质子耦合的失电子过程逐步生成高价态的金属-氧物种, 其引发的O-O成键过程通常是水氧化催化循环的决速步骤. 基于之前的研究成果, 目前主要报道了五种不同的O-O成键机理: (1)水亲核进攻金属-氧物种的WNA机理, (2)金属-氧自由基耦合的I2M机理, (3)金属-羟基自由基耦合的HC机理, (4)分子内进攻桥连氧的IOC机理以及(5)氧化还原异构的RI机理.
本文综述了过去几十年水氧化分子催化剂的发展, 总结了贵金属钌和铱配合物到第一过渡金属锰、铁、钴、镍和铜配合物催化水氧化过程中金属-氧物种的生成与演化, 重点阐述了引发O-O成键过程的高价态金属-氧物种的种类及其不同的O-O成键机理. 重点总结了O-O成键中WNA机理与I2M机理的异同, 并阐述了催化剂设计对WNA与I2M机理选择性的影响. 通过对金属-氧物种种类和O-O成键机理的总结, 将有助于进一步设计合成高效稳定的水氧化分子催化剂.

关键词: 产氧反应, 水氧化, O-O成键, 过渡金属配合物, 分子电催化, 反应机理

Abstract:

Water oxidation is one of the most important reactions in natural and artificial energy conversion schemes. In nature, solar energy is converted to chemical energy via water oxidation at the oxygen-evolving center of photosystem II to generate dioxygen, protons, and electrons. In artificial energy schemes, water oxidation is one of the half reactions of water splitting, which is an appealing strategy for energy conversion via photocatalytic, electrocatalytic, or photoelectrocatalytic processes. Because it is thermodynamically unfavorable and kinetically slow, water oxidation is the bottleneck for achieving large-scale water splitting. Thus, developing highly efficient water oxidation catalysts has attracted the interests of researchers in the past decades. The formation of O-O bonds is typically the rate-determining step of the water oxidation catalytic cycle. Therefore, better understanding this key step is critical for the rational design of more efficient catalysts. This review focuses on elucidating the evolution of metal-oxygen species during transition metal-catalyzed water oxidation, and more importantly, on discussing the feasible O-O bond formation mechanisms during the oxygen evolution reaction over synthetic molecular catalysts.

Key words: Oxygen evolution reaction, Water oxidation, O-O bond formation, Transition metal complex, Molecular electrocatalysis, Reaction mechanism

张学鹏, 王红艳, 郑浩铨, 张伟, 曹睿. 分子催化剂催化水氧化过程及其O-O成键机理[J]. 催化学报, 2021, 42(8): 1253-1268.

Xue-Peng Zhang, Hong-Yan Wang, Haoquan Zheng, Wei Zhang, Rui Cao. O-O bond formation mechanisms during the oxygen evolution reaction over synthetic molecular catalysts[J]. Chinese Journal of Catalysis, 2021, 42(8): 1253-1268.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(20)63681-6

https://www.cjcatal.com/CN/Y2021/V42/I8/1253

图/表 27

Scheme 1. Schematic diagrams of proposed O-O bond formation mechanisms: (a) water nucleophilic attack (WNA), (b) coupling between two metal oxo/oxyl units (I2M), (c) bimolecular hydroxyl coupling (BHC), (d) intramolecular hydroxyl coupling (IHC), (e) intramolecular coupling between hydroxyl and bridging oxo (intermolecular oxo/oxyl coupling; IOC), and (f) coupling between two bridging oxo units (redox isomerization; RI).

Scheme 2. Molecular structure of 1 blue dimer, where bpy denotes bipyridine, and proposed oxo-bridged binuclear Ru complex-mediated water nucleophilic attack O-O bond formation mechanism.

Scheme 3. Molecular structure of 2 and proposed water oxidation catalytic cycle

Scheme 4. Molecular structure of 3, and water nucleophilic attack (WNA) and intramolecular oxo/oxyl coupling (IOC) O-O bond formation pathways.

Scheme 5. Molecular structures of 4 and 5, and their respective key intermediates that are nucleophilically attacked by solvent H2O molecules.

Scheme 6. Molecular structure of 6 and water nucleophilic attack of the RuV=O moiety.

Scheme 7. Proposed catalytic cycle of mononuclear Ru-mediated water oxidation; the O-O bond formation mechanism follows the water nucleophilic attack (WNA) pathway.

Scheme 8. Molecular structure of 7 and schematic of base-assisted solvent H2O nucleophilic attack of the IrV=O moiety.

Scheme 9. Molecular structures of 8 and 9. Proposed water nucleophilic attack (WNA) pathway of O-O bond formation, which involved the participation of an outer-sphere H2O molecule or the [CeIV(NO3)3(OH)] complex.

Scheme 10. Molecular structures of 10, 11, 12 and 13, and proposed 11-mediated water nucleophilic attack (WNA)-type water oxidation catalytic cycle.

Scheme 11. Molecular structure of 14, and proposed hangman-assisted water nucleophilic attack (WNA)-type O-O bond formation mechanism.

Scheme 12. Molecular structure of 15, and schematic diagram of two different water nucleophilic attack-type O-O bond formation transition states using a H2O cluster or an acetate anion as the external bases.

Scheme 13. Molecular structure of 16 and proposed water oxidation catalytic cycle.

Scheme 14. Molecular structure of 17, and proposed water oxidation catalytic cycle via single electron transfer (SET)-water nucleophilic attack O-O bond formation.

Scheme 15. Molecular structures of 18, and proposed coupling between two metal oxo/oxyl units (I2M)-type O-O bond formation mechanism.

Scheme 16. Molecular structures of 19 and 20, and proposed 19-mediated intramolecular coupling between two metal oxo/oxyl units (I2M)-type O-O bond formation mechanism.

Scheme 17. (a) Molecular structure of 21. (b) Isolated seven-coordinated Ru(IV) dimer complex with [H2O-HO-H-OH-H2O]- bridge. (c) Intramolecular coupling between two metal oxo/oxyl units (I2M) O-O bond formation mechanism between two seven-coordinated RuV=O (or RuIV-O?) intermediates.

Scheme 18. Molecular structure of 22, and π-π stacking noncovalent interaction between two isoquinoline moieties.

Scheme 19. Schematic diagram of origins of different O-O bond formation mechanism mediated by 23 and 24.

Scheme 20. Schematic diagram of origins of different O-O bond formation mechanism mediated by 25 and 26.

Scheme 21. Molecular structures of 27 and 28, and proposed water nucleophilic attack (WNA) or coupling between two metal oxo/oxyl units (I2M) O-O bond formation mechanisms.

Scheme 22. Molecular structure of 29, and proposed mechanism for the formation of H2 and O2 from H2O.

Scheme 23. Molecular structures of 30 and 31 and their respective key intermediates for hydroxyl coupling O-O bond formation.

Scheme 24. Molecular structure of 32 and the proposed catalytic cycle of water oxidation.

Scheme 25. Molecular structure of 33 and the two different O-O bond formation mechanisms of WNA and IOC.

Scheme 26. Molecular structure of 34 and the proposed O-O bond formation mechanism via an IOC mechanism.

Scheme 27. Molecular structure of 35 and the proposed O-O bond formation mechanism via either a RI or a WNA strategy.

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分子催化剂催化水氧化过程及其O-O成键机理

O-O bond formation mechanisms during the oxygen evolution reaction over synthetic molecular catalysts

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