Theoretical understanding of electrocatalysis beyond thermodynamic analysis

doi:10.1016/S1872-2067(22)64090-7

Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (11): 2746-2756.DOI: 10.1016/S1872-2067(22)64090-7

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Theoretical understanding of electrocatalysis beyond thermodynamic analysis

Huan Li^a^,^b, Chenxi Guo^a, Jun Long^a^,^c, Xiaoyan Fu^a^,^c, Jianping Xiao^a^,^b^,^d^,^*()

^aState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^bUniversity of Chinese Academy of Sciences, Beijing 100049, China
^cDepartment of Chemistry, Zhejiang University, Hangzhou 310058, Zhejiang, China
^dState Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2022-02-22 Accepted:2022-04-21 Online:2022-11-18 Published:2022-10-20
Contact: Jianping Xiao
About author:Jianping Xiao (Dalian Institute of Chemical Physics, Chinese Academy of Science) received his B.A. degree from Chongqing University (China) in 2007, and Ph.D. degree from Bremen University (Germany) in 2013. He worked as a postdoctoral researcher in Dalian Institute of Chemical Physics, Chinese Academy of Sciences from 2013 to 2015. Since the end of 2015, he moved and worked at Stanford University (USA) until the end of 2017. He was awarded with National Youth Talents (2019) and Mercator Fellow from DFG, Germany (2021). His research interests mainly focus on the theory and simulation of heterogeneous catalysis and electrocatalysis, especially reaction phase diagram and anomalous activity and selectivity trend. He has published more than 90 peer-reviewed articles.
Supported by:
National Key Research and Development Program of China(2021YFA1500702);National Natural Science Foundation of China(22172156);National Natural Science Foundation of China(91945302);DNL Cooperation Fund, CAS(DNL202003);Liaoning Revitalization Talents Program(XLYC1907099);Strategic Priority Research Program of the Chinese Academy of Sciences(XDB36030200)

Abstract

Abstract:

As the green and sustainable development of human society highly relies on renewable energy, it has been recognized that electrocatalysis is a key technology to this end. High efficient ways of carbon-neutralization (eCO₂RR), reverse artificial nitrogen cycle (RANC), and oxygen chemistry (OER and ORR) all can be driven by electrocatalysis. Advanced theoretical study is an important means to fundamentally understanding electrocatalytic reactions. Herein, we review a few significant issues in theoretical electrocatalysis. First, electrochemical barriers and potential effects are essential for a more accurate description of reaction mechanism and activity. Meanwhile, consideration of competitive reaction path is also one of the important aspects, as novel insights and anomalous volcano trend can be obtained. Finally, a microenvironment exerted by confined space can tune the capacitance of electrochemical interface and (electro)chemical potential of proton, resulting in a possibility to improve reaction activity, which opens a new avenue for design of catalyst.

Key words: Electrocatalysis, Capacitor model, Potential-dependent barrier, Anomalous volcano, Confinement

Huan Li, Chenxi Guo, Jun Long, Xiaoyan Fu, Jianping Xiao. Theoretical understanding of electrocatalysis beyond thermodynamic analysis[J]. Chinese Journal of Catalysis, 2022, 43(11): 2746-2756.

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Figures/Tables 9

Scheme 1. Schematic view of green and sustainable energy landscape based on electrocatalysis, where eCO2RR, RANC, and oxygen electrochemistry (OER and ORR) are highlighted in green, blue and red, respectively.

Fig. 1. (a) Local atomic structures of IS, TS, and FS for monolayer and multilayer (i) models. The light blue, blue, red, and white atoms are Ag, N, O, and H, respectively. The green atom is the transferred proton. (b) Extrapolated electrochemical barriers plotted against work function (Φ) for Volmer and NO protonation reactions using monolayer and multilayer water structures on Ag(111). Reprinted with permission from Ref. [45]. Copyright 2021, American Chemical Society.

Fig. 2. Free energy diagrams for eNORR to NH3 (a) and HER (b) at low potentials, where the subfigures show the potential-dependent barriers of corresponding potential-determining steps (PDSs), calculated with a monolayer (circle) and multilayer (triangle) water structure. Theoretical (c) and experimental (d) Faradaic efficiencies of different products on Ag. Reprinted with permission from Ref. [45]. Copyright 2021, American Chemical Society.

Fig. 3. (a,b) Calculated charge transfer (Δq, the surface charge of final states was set as reference to be 0) and work function (Φ) on the surfaces at IS, TS and FS for electrochemical processes in OER, including reaction of O* coupling with deprotonated H2O (a) and OOH* deprotonation step (b). (c) Free energy diagram, with potential-dependent activation barriers for each elementary step, for OER over Co2MnO4 at 1.23 and 1.70 V vs. RHE. (d) Comparison between the experimental current (log(j)) and theoretical rate (log(TOF)) calculated by microkinetic modelling on Co2MnO4 at various electrode potentials. Reprinted with permission from Ref. [48]. Copyright 2021, Springer Nature.

Fig. 4. (a) The scheme of potential-dependent β and reaction energy diagrams for a proton-electron coupled transfer step (A* + (H+ + e-) → AH*) at different potential in subFig.s, where the atomic models schematically show the IS-like and FS-like transition states. (b) Schematic charge transfer (Δq) and work function (Φ) on the surfaces at IS, TS and FS for A* + (H+ + e-) → AH* step. Note that Δq and Φ of TS will alter between FS and IS along coordinates of work function.

Fig. 5. (a) The one-dimensional reaction phase diagram (RPD) for CO2RR, where the solid lines show the GRPD-limiting steps for the more favored COOH* path (red) and the HCOO* path (blue). (b) Comparison between the theoretical descriptor of activity (-GRPD-limiting) and the experimental activity (log[-j(A?cm-2)]). The dashed line shows the correlation between experimental and theoretical activity, which is described by the GRPD-limiting energy of the more favored path through either COOH* or HCOO*. Reprinted with permission from Ref. [56]. Copyright 2021, Springer Nature.

Fig. 6. (a-c) Comparison of potential-turnover frequency (TOF) from microkinetic modelling between electrochemical (blue) and thermochemical (black) steps in O2* (a), OOH* (b) and O* (c) conversion. (d) Theoretical activity (log(i)) based on microkinetic modeling with the fitted Tafel slopes at the high and low electrode potential based on the experiments (insert Figure). (e) GRPD-limiting steps for two-dimensional RPD with the descriptor of EadO* and EadOH* at 0.5 V vs. RHE displayed in different colors with the color bar on the right. The reactions from R1 to R8 are O2(g) + * ↔ O2*, O2* + * ↔ 2O*, OOH* + * ↔ OH* +O*, H2O(l) + O* + * ↔ 2OH*, O* + (H+ + e-) ↔ OH*, OH* + (H+ + e-) ↔ H2O(l) + *, O2* + (H+ + e-) ↔ OOH* and OOH* + (H+ + e-) ↔ H2O(l) + O*. (Potential-dependent two-dimensional RPDs at different electrode potentials of 0.5 V (f), 0.7 V (g), and 0.9 V (h) vs. RHE. The peak of the GRPD activity trend at different electrode potentials was showed as a triangle (0.5 V), circle (0.7 V), and square (0.9 V). The GRPD were showed relevant to the color bar on the right. The data was adopted with permission from Ref. [59]. Copyright 2020, American Chemical Society.

Fig. 7. Competition between N2O and NH3 production in eNORR, at high potentials. (a) Degree of rate control of different elementary steps (XRC) for N2O production. (b) Theoretical reaction rate for N2O and NH3 production, where “n” is the electron transfer number for corresponding total reactions. The inset Fig. shows the partial current densities (jpar) from experiment, obtained with the equation jpar = jtot × FE, where “jtot” is the total current density. Reprinted with permission from Ref. [45]. Copyright 2021, American Chemical Society.

Fig. 8. Calculated charge transfer (Δq) and potential variation at IS and TS with respect to FS of Volmer (a) and Heyrovsky (b) steps in HER; Calculated potential-dependent forward reaction energies (ΔE), forward kinetic barriers (Ea), and backward kinetic barriers (Eb) on Cu(211) surface for Volmer (c) and Heyrovsky (d) reactions, in confined nanoscale reactors. (e) Micro-kinetic modeling of HER with the Volmer and Heyrovsky path. The pink and blue lines are the TOFs of reactions on the open Cu(211) and Cu(211) with graphene cover, respectively. (f) Scheme of confinement energy (Econ) formation, resulting in more favorable reaction energies and lower electrochemical kinetic barrier. Econ is defined as the difference between an open system (red dots) and the confined electrochemical system (blue dots), which is composed of two components including the enhanced (electro)chemical potential of the proton and weakening the adsorption energies of adsorbates. Reprinted with permission from Ref. [63]. Copyright 2019, American Chemical Society.

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Theoretical understanding of electrocatalysis beyond thermodynamic analysis

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