脉冲电催化的研究进展及性能强化机制

doi:10.6023/A22080342

化学学报 ›› 2022, Vol. 80 ›› Issue (11): 1555-1568.DOI: 10.6023/A22080342 上一篇

综述

脉冲电催化的研究进展及性能强化机制

王金格, 周伟^*(), 李佳轶, 丁雅妮, 高继慧

哈尔滨工业大学能源科学与工程学院哈尔滨 150001

投稿日期:2022-08-03 发布日期:2022-09-19
通讯作者: 周伟

作者简介:

王金格, 女, 哈尔滨工业大学能源科学与工程学院硕士研究生, 主要研究方向为脉冲电催化合成过氧化氢.

周伟, 2019年于哈尔滨工业大学获得博士学位, 期间于2016~2018年受国家留学基金委资助在美国东北大学进行联合培养. 现任哈尔滨工业大学青年拔尖副教授, 博士生导师. 主要致力于低电耗重质碳辅助电解水制氢、脉冲电催化过氧化氢合成及基于羟基自由基的高级氧化技术等研究. 在Appl. Catal. B-environ., J. Mater. Chem. A, Chem. Eng. J., Adv. Mater. Interfaces等学术刊物上发表论文60余篇, 相关研究被引用900余次. 主持国家自然科学基金青年项目、中国博士后基金特别资助项目、中国博士后基金面上项目、黑龙江省博后基金(一等)等多项科研项目.

李佳轶, 男, 哈尔滨工业大学能源科学与工程学院硕士研究生, 主要研究方向为木质素辅助电解水制氢.

丁雅妮, 女, 博士研究生, 现就读于哈尔滨工业大学能源科学与工程学院. 主要研究方向为脉冲动态电催化、ORR界面能质传递动态调控、杂原子掺杂碳基电催化剂设计及电催化高级氧化技术. 以第一作者及共同作者于Appl. Catal. B-environ., J. Mater. Chem. A, Adv. Mater. Interfaces, Chem. Eng. J.等期刊上发表SCI论文10余篇, 被引用次数300余次.

高继慧, 哈尔滨工业大学教授, 教育部创新创业教育指导委员会委员, 获国家技术发明二等奖2项、省部级科技奖励3项; 主持及组织完成国家科技部项目5项、自然科学基金重点项目及面上10余项, 发表学术论文160余篇, 申请及授权国家发明专利60余项.

基金资助:
哈尔滨工业大学城市水资源与水环境国家重点实验室开放基金(QG202229)

Recent Advances and Performance Enhancement Mechanisms of Pulsed Electrocatalysis

Jinge Wang, Wei Zhou(), Jiayi Li, Yani Ding, Jihui Gao

School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, China

Received:2022-08-03 Published:2022-09-19
Contact: Wei Zhou
Supported by:
Open Project of State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology(QG202229)

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摘要/Abstract

基于电催化的能源转化、化学品合成及污染物降解技术是解决能源与环境问题的重要方式. 一些研究已经证明, 通过简单地施加周期性切换电位的脉冲供电策略, 将会有效提升电催化性能. 本文对脉冲供电策略在电化学高级氧化、电化学二氧化碳还原、有机电合成、电解水制氢等经典电化学体系中的应用及研究进展进行了综述, 并具体分析了其对各类电催化反应性能的强化机制, 这些机制主要包括: 通过周期性更新能斯特扩散层的物质浓度以增强催化活性; 通过动态调控中间体吸附能以提高催化选择性; 通过维持催化剂表面处于非平衡状态, 避免催化剂失活以提高催化剂的稳定性. 最后, 本文展望了脉冲电催化未来所面临的机遇与挑战.

关键词: 脉冲电催化, 电化学高级氧化, 电化学二氧化碳还原, 有机电合成, 电解水制氢

Due to the excessive exploitation and utilization of fossil fuels, we are faced with severe energy and environmental problems. Therefore, it's significant to develop electrocatalytic energy conversion, chemical synthesis and pollutant degradation technologies. In order to achieve high activity, selectivity and stability of electrocatalytic reactions, researchers have made a lot of efforts in catalyst design, interface microenvironment regulation and reactor structure optimization. In fact, there is still a wide space on the power supply side for the regulation of electrocatalytic system. Although most researchers choose to use potentiostatic or galvanostatic power supply strategy, some studies have proven that the pulsed power supply strategy by implementing altering potential periodically can improve electrocatalytic performance to a great extent. Compared with traditional regulating methods mentioned above, the pulsed electrocatalysis is much simpler, efficient and repeatable because it just needs to modulate the output potential or current mode. In addition, it is more favorable to be coupled with smart energy in the future. Therefore, the pulsed electrocatalysis has broad development prospects. In this review, we summarized the application and recent progress of the pulsed power supply strategy in classical electrocatalytic systems include electrochemical advanced oxidation processes, electrochemical carbon dioxide reduction, organic electrochemical synthesis, hydrogen production through water electrolysis. Besides, we analyzed the enhancement mechanisms of pulsed electrocatalysis. These enhancement mechanisms can be generalized as follows: (1) By updating the concentration of substance in Nernst diffusion layer during the implementation of switching potential periodically, the concentration polarization can be prevented. Thus, the electrocatalytic activity can be enhanced. Besides, some side reactions caused by mass transfer restriction can also be suppressed. (2) Through altering the adsorption energy of the reaction intermediate and adjusting the coverage of intermediate on the catalyst surface under oscillating potential periodically, the electrocatalytic selectivity of target reaction can be increased. Furthermore, because the active site of catalyst can be modulated to alternate between ideal states for adsorption of intermediate and desorption of product, the Sabatier's theoretical limit on static catalytic site may be breached and the turnover frequency (TOF) of the catalyst can increase by several orders of magnitude during the pulsed dynamic electrocatalysis process. (3) The catalyst surface can be kept in a non-equilibrium state to avoid the inactivation caused by excessive oxidation or reduction of active site or the deposition of some toxic substances on the surface of a catalyst. Thus, the electrocatalytic stability will be improved. Besides, the dynamic reconfiguration of catalysts during pulsed electrocatalysis will influence the activity and selectivity of reaction. Finally, we prospect for the challenges and opportunities of pulsed electrocatalysis in the future.

Key words: pulsed electrocatalysis, electrochemical advanced oxidation, electrochemical carbon dioxide reduction, organic electrochemical synthesis, electrolysis of water to produce hydrogen

引用此文

王金格, 周伟, 李佳轶, 丁雅妮, 高继慧. 脉冲电催化的研究进展及性能强化机制[J]. 化学学报, 2022, 80(11): 1555-1568.

Jinge Wang, Wei Zhou, Jiayi Li, Yani Ding, Jihui Gao. Recent Advances and Performance Enhancement Mechanisms of Pulsed Electrocatalysis[J]. Acta Chimica Sinica, 2022, 80(11): 1555-1568.

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图/表 9

图1. 本文整体框架图

Figure 1. The overall frame diagram of this paper

图2. 周期性切换电位的脉冲供电模式: (a) 交替施加阳极电位和静息电位的阳极单脉冲模式; (b) 交替施加阴极电位和静息电位的阴极单脉冲模式; (c) 交替施加阳极电位和阴极电位的双脉冲模式

Figure 2. Pulse power supply mode with periodic switching potential: (a) anode single pulse power supply mode with alternating anodic potential and rest potential; (b) cathode single pulse power supply mode with alternating cathode potential and rest potential; (c) double pulse power supply mode with alternating anodic and cathodic potentials

图3. 在不同阳极脉冲时间ta和阴极脉冲时间tc组合(Ec=-1.0 V vs. RHE, Ea=＋0.6 V vs. RHE)下Cu NCs催化剂的表面氧化态及对应的产物选择性[29]: (a) 在tc>>ta时, 催化剂表面几乎完全呈金属态, 并且P-ECO2RR的产物中C2H4的FE最大; (b) 在tc<<ta时, 催化剂表面形成了较厚的Cu2O壳层, 这促进了CO和CH4的生成; (c) 在ta值较低且tc值中等时, 催化剂表面氧化态和还原态铜物种的平衡促进了乙醇的生成

Figure 3. Surface oxidation state and product selectivity of Cu NCs catalyst at different combinations of anode pulse time ta and cathode pulse time tc (Ec=-1.0 V vs. RHE, Ea=＋0.6 V vs. RHE)[29]: (a) at tc>>ta, the surface of the catalyst is almost completely metallic and C2H4 has the largest FE in the products of P-ECO2RR; (b) at tc<<ta, the formation of a thicker Cu2O shell on the catalyst surface results in an enhanced CO and CH4 formation; (c) at low ta and intermediate tc values, the balance between oxidized and reduced copper species on the catalyst surface results in an enhanced ethanol formation Adapted with permission from Ref. [29]. Copyright 2022, Nature Publishing Group.

图4. 在tc=25 s, ta=5 s, Ec=-1.6 V, Ea如图中注明的脉冲条件下电解16 h后, 铜片电极表面的扫描电子显微镜图像(放大倍数为20000×)[78]

Figure 4. SEM images of copper sheet electrode surfaces after 16 h electrolysis with tc=25 s, ta=5 s, Ec=-1.6 V, and Ea as noted in each image (magnification 20000×)[78] Adapted with permission from Ref. [78]. Copyright 2018, IOP Publishing Ltd.

图5. pH的增加和CO2浓度的积累对C2＋产物选择性提高的促进作用[27]: (a) 在0.1 mol/L CsHCO3溶液中Cu上进行的P-ECO2RR的时间依赖连续模型的模拟结果; (b) 脉冲与恒电位条件下产物选择性的比较

Figure 5. The enhanced pH and the accumulation of CO2 concentration promoted the selectivity of C2＋ products[27]: (a) the results of the time-dependent continuum model of P-ECO2RR simulation on Cu in 0.1 mol/L CsHCO3; (b) comparison of product selectivity under pulsed and potentiostatic condition Adapted with permission from Ref. [27]. Copyright 2020, American Chemical Society

图6. P-ECO2RR期间Cu表面OHads吸附中间体覆盖率的增加对C2产物选择性的增强作用[28]: (a) 在阳极脉冲期间, Cu表面的质子受到排斥作用并被氢氧化物置换, 表面残留的氢氧化物与邻近的CO发生偶联作用, 有利于生成C2产物; (b) 先在脉冲电位(Ec=-1.05 V, Ea=＋0.4 V, tc=ta=50 ms)下电解, 再切换到恒电位(E=-1.05 V)持续电解1.5 h, 最后切换回起始脉冲电位电解时, CO2还原的主产物(蓝色)和H2(红色)的FE随时间的变化情况

Figure 6. The increased coverage of OHads adsorption intermediates on Cu surface during P-ECO2RR enhanced the selectivity of C2 products[28]: (a) the surface protons will be repelled and displaced by hydroxides during the anodic pulse and the remaining surface hydroxides will induce near neighbor coupling with CO, favoring C2 products during the cathodic potential; (b) FE of major ECO2RR reduction products (blue) and H2 (red) over time, starting with a pulsed potential (Ec=-1.05 V, Ea=＋0.4 V, tc=ta=50 ms), then switching to a constant potential (E=-1.05 V) for 1.5 h and finally switching back to the starting pulsed potential Adapted with permission from Ref. [28]. Copyright 2020, American Chemical Society

图7. 传统手性电合成与脉冲手性电合成的比较[35]: 在使用手性编码铂电极的传统与脉冲不对称电合成过程中, 通过立体选择性加氢(绿色点)将非手性苯乙酮(黄色点)转化为(R)-和(S)-PE(蓝色点和红色点)

Figure 7. Comparison of conventional and pulsed chiral electrosynthesis[35]: conversion of achiral acetophenone (yellow dots) into (R)- and (S)-PE (blue and red dots, respectively) by stereoselective addition of hydrogen (green dots) during conventional and pulsed asymmetric electrosynthesis using chiral-encoded Pt electrodes Adapted with permission from Ref. [35]. Copyright 2017, Nature Publishing Group

图8. 交替电极极性的脉冲策略对有机电合成传质过程的影响[110,112]: (a) 配对电解(左)和用于包括两个相反氧化还原步骤的连续反应的交替电极极性的脉冲电解(右); (b) 依赖物质输运的常规电解(左)和通过在两个电极上形成中间体来避免物质输运限制的脉冲电解(右)

Figure 8. Effect of pulsed strategy by alternating electrode polarity on mass transfer in OES[110?-112]: (a) paired electrolysis (left) and pulsed electrolysis of alternating electrode polarity for a sequential reaction that includes two redox-opposite steps (right); (b) normal electrolysis dependent on mass transport (left) and pulsed electrolysis avoiding the limit of mass transport by forming intermediates on both electrodes (right) (a) Adapted with permission from Ref. [110]. Copyright 2020, American Chemical Society. (b) Adapted with permission from Ref. [112]. Copyright 2021, the Royal Society of Chemistry

图9. 甲酸在Pt上动态电催化分解的反应能及反应途径[31]: (a) 甲酸在铂上的分解通过初始的非法拉第分解进行热力学下坡过程, 生成水和吸附态CO* (ΔE=-2 eV), 随后CO*氧化为CO2 (g)的法拉第过程通过放出能量或吸收能量的可调节活化能的途径进行, 活化能依赖于施加电位; (b) 施加的电位在有利于非法拉第过程中甲酸分解的开路电位和有利于吸附态CO*的电催化氧化的电位(0.8 V)之间动态振荡, 从而提高了催化循环的速率

Figure 9. Reaction energies and pathways of dynamic formic acid electrocatalytic decomposition on Pt[31]: (a) the decomposition of formic acid on Pt proceeds thermodynamically downhill through an initial nonfaradic decomposition to water and adsorbed CO* (ΔE=-2 eV). The subsequent faradaic oxidation of CO* to CO2(g) proceeds via exergonic or endergonic pathways with tunable activation energy dependent on the applied potential; (b) the catalytic cycle proceeds at enhanced rates via dynamic oscillation of the applied potential between open circuit, which is favorable to nonfaradaic formic acid decomposition, and 0.8 V, which is favorable for electrocatalytic oxidation of adsorbed CO* Adapted with permission from Ref. [31]. Copyright 2020, American Chemical Society

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脉冲电催化的研究进展及性能强化机制

Recent Advances and Performance Enhancement Mechanisms of Pulsed Electrocatalysis

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