The dynamic behaviors of heterogeneous interfaces in electrocatalytic CO2 reduction

doi:10.1016/S1872-2067(23)64543-7

Abstract

Abstract:

The electrocatalytic CO₂ reduction reaction (CO₂RR) is a highly promising renewable energy technology that can convert greenhouse gases into valuable fuels and chemicals. However, under ordinary operating conditions, significant dynamic evolution behavior occurs on the catalyst surface, which is mainly manifested as surface morphology evolution and property changes, eventually leading to changes in the active sites of the reaction, affecting selectivity and efficiency. To develop efficient electrocatalytic systems with excellent performance, an essential prerequisite is to understand the underlying mechanism of surface dynamic evolution. Studying the influence of the external environment on dynamic evolution is as important as studying the intrinsic structural properties of catalysts. In this review, we first introduce the concept of dynamic evolution and then emphasize the influence of the external environment (applied potential, temperature, electrolyte, and impurities) on CO₂RR dynamic evolution. We also address the use of operando characterization techniques and pulsed CO₂ electrolysis methods for monitoring and controlling dynamic evolution behaviors under working conditions, along with theoretical methods, including ab initio calculations and machine learning that can simulate dynamic behavior. Finally, we present several current challenges and prospects for the development of techniques for controlling the CO₂RR dynamic evolution.

Key words: CO₂ reduction reaction, Dynamic behavior, Active site, External environment, Electrocatalysis

Shenyu Shen, Qingfeng Guo, Tiantian Wu, Yaqiong Su. The dynamic behaviors of heterogeneous interfaces in electrocatalytic CO₂ reduction[J]. Chinese Journal of Catalysis, 2023, 53: 52-71.

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Figures/Tables 12

Fig. 1. (a) HAADF-STEM images and EDS elemental mapping of intermixed AgCu catalysts after the CO2RR has proceeded for 0, 0.5, 1, 3, 6, and 24 h. Scale bars in the top row, 50 nm; bottom row, 20 nm. Reprinted with permission from Ref. [25]. Copyright 2023, American Chemical Society. (b) Structural evolution of CuSiOx and CuO before and after the CO2RR at -1.4 V vs. RHE for 2 h. (c,d) Faradaic efficiencies (FEs) of the CO2RR products on CuO and CuSiOx at different potentials. Reprinted with permission from Ref. [27]. Copyright 2023, American Chemical Society. (e) TEM image after the introduction of Cu2O NPs of size 20 nm. (f) HRTEM image of Cu-based NPs after the CO2RR has proceeded for 10 h. (g) FEs of CO2RR products on fragmented Cu-based NP/C at different potentials. Reprinted with permission from Ref. [29]. Copyright 2019, American Chemical Society.

Fig. 2. (a) XANES spectra of Cu(pc) in CO2-saturated 0.1 mol L-1 KHCO3 as a function of the applied potentials. (b) EXAFS spectra of Cu(pc) thin-film electrode. Reprinted with permission from Ref. [31]. Copyright 2021, American Chemical Society. (c) EXAFS spectra of as-prepared Zn NPs. (d) EXAFS spectra of Zn NPs during CO2RR. Reprinted with permission from Ref. [38]. Copyright 2018, American Chemical Society. (e,f) The trend of methanol production and coordination numbers of In-O and In-In changes with the variation of TOS (time on stream). Reprinted with permission from Ref. [40]. Copyright 2019, American Chemical Society.

Fig. 3. High-resolution transmission electron microscopy (HR-TEM) images of ET-H (+1.2 VRHE) (a) and ET-L (+0.8 VRHE) (b) catalysts. ET refers to electrochemical treatment. The grain boundaries are highlighted with red lines. Reprinted with permission from Ref. [50]. Copyright 2022, American Chemical Society. (c) Grand free energy profiles of CO2 activation on Cu(100) through the SEPT and CPET mechanisms. Reprinted with permission from Ref. [54]. Copyright 2023, American Chemical Society. (d) Electrochemical scanning tunneling microscopy (EC-STM) images of polycrystalline copper surface at -0.9 V in 0.1 mol L-1 KOH. Reprinted with permission from Ref. [52]. Copyright 2014, American Chemical Society.

Fig. 4. Faradaic efficiency (in dark circles) and partial current density (in light squares) during CO2RR at different reaction temperatures in 0.1 mol L-1 KHCO3 at ?1.1 V vs. RHE for C2H4 (a) and H2 (b). (c) Carbon efficiency towards CO at ?1.1 V vs. RHE. SEM micrographs after CO2RR at -1.1 V vs. RHE at 25 °C (d), 48 °C (e) and 70 °C (f). Reprinted with permission from Ref. [61]. Copyright 2023, American Chemical Society.

Fig. 5. (a) CO2RR in 0.2 mol L-1 phosphate buffers with pH values of 1 and 7 on Cu(111) and Cu(100). Reprinted with permission from Ref. [82]. Copyright 2013, Elsevier. (b) Surface Pourbaix diagram under global thermodynamic equilibrium. The color bar represents the H coverage (in ML). (c) Root-mean-square deviation (RMSD) of the top-layer Cu positions during equilibrated 10 ps Born-Oppenheimer molecular dynamics (BOMD) simulations of the unrestructured surface with 0-, 1/6-, and 1/3-ML H coverage. (d) Key snapshots during an equilibrated 10 ps BOMD simulation of the 12 H state with an unrestructured initial configuration (the shifting row is highlighted by green or blue, before or after the shift). Reprinted with permission from Ref. [84]. Copyright 2022, American Chemical Society. (e) STEM-HAADF image of the surface of a Cu2O nanocube. The different atomic structures are labeled by regions I and II. Reprinted with permission from Ref. [41]. Copyright 2022, Elsevier. Time- and potential-dependent sequences of EC-STM images of Cu(111) at a pH of 13 (f) and 11 (g). Reprinted with permission from Ref. [86]. Copyright 2021, American Chemical Society.

Fig. 6. (a) The activity of CO generation in the presence of different cations. Reprinted with permission from Ref. [87]. Copyright 2021, American Chemical Society. (b,c) CV of the platinum ultramicroelectrode (Pt-UME) after CO2RR on gold and silver electrodes. Reprinted with permission from Ref. [88]. Copyright 2021, Springer Nature. (d-f) The partial current densities of the main products on Cu(100) in the presence of different cations. Reprinted with permission from Ref. [90]. Copyright 2017, American Chemical Society. (g-i) SEM images of electropolished Cu (EP-Cu), oxidized Cu (Ox-Cu), and Re-Cu-I. (j) FE of C2 products on Re-Cu-I, Re-Cu-Br, Re-Cu-Cl, and EP-Cu at different potentials. Reprinted with permission from Ref. [94]. Copyright 2020, Royal Society of Chemistry.

Fig. 7. (a) Pd-induced surface restructuring strategy. Reprinted with permission from Ref. [98]. Copyright 2017, John Wiley and Sons. (b,c) FEs of CO2RR products of pure CO2 and CO2/O2 at different applied potentials. Reprinted with permission from Ref. [107]. Copyright 2016, Elsevier. (d) BF-TEM image of Cu catalyst after electrolysis in CO2 + SO2 experiment. Reprinted with permission from Ref. [108]. Copyright 2019, American Chemical Society.

Fig. 8. (a) IR spectra at different applied potentials on Ag catalyst in CO2-saturated 0.1 mol L-1 KCl electrolyte. Reprinted with permission from Ref. [9]. Copyright 2017, American Chemical Society. (b,c) In situ SERS of Cu surface in CO2-saturated 0.1 mol L-1 KHCO3. Reprinted with permission from Ref. [121]. Copyright 2021, John Wiley and Sons. (d) A schematic of the developed operando Raman measurement system. (e) Operando Raman spectra of the peroxo O-O band evolution. Reprinted with permission from Ref. [122]. Copyright 2022, American Chemical Society.

Fig. 9. (a) In situ In K-edge XANES of InZr_7.1 at different temperatures in CO2 or reaction atmosphere. (b) The corresponding Fourier transformed EXAFS spectra of InZr_7.1. Reprinted with permission from Ref. [125]. Copyright 2019, American Chemical Society. (c,d) In situ XPS spectra of the Cu 2p3/2 and Zn 2p3/2 core level regions before and after 1 h of CO2RR. Reprinted with permission from Ref. [126]. Copyright 2019, American Chemical Society. (e) XRD patterns of intermixed AgCu particles after CO2RR. Reprinted with permission from Ref. [25]. Copyright 2023, American Chemical Society.

Fig. 10. (a) STEM-HAADF images of the morphology of Cu2O nanocubes at different stages. Reprinted with permission from Ref. [41]. Copyright 2022, Elsevier. (b,c) In situ EC-AFM images of electropolished Cu(100) surface at -0.5 and -1.0 V vs. RHE. Reprinted with permission from Ref. [57]. Copyright 2020, John Wiley and Sons. (d-f) AFM images that depict the surface morphologies of EP-Cu, E-ID-Cu and W-ID-Cu. Reprinted with permission from Ref. [129]. Copyright 2023, John Wiley and Sons.

Fig. 11. (a) FEs of CO2RR products on Cu electrode at constant potential and pulsed potential with different cathodic intervals (tc) and anodic intervals (ta). Reprinted with permission from Ref. [120]. Copyright 2018, John Wiley and Sons. (b) FEs of CO2RR products on Cu electrodes at constant potential and pulsed potential in a 0.1 mol L-1 KHCO3 electrolyte and a 0.1 mol L-1 KCl electrolyte. Reprinted with permission from Ref. [138]. Copyright 2020, John Wiley and Sons. (c-e) AFM images of Cu(100) electrode at constant potential and pulsed potential for different anodic potentials. Reprinted with permission from Ref. [131]. Copyright 2020, Springer Nature.

Fig. 12. (a,b) Grand potential interface energies of Cu surfaces with the adsorption of H and CO. (c) pH- and potential-dependent Wulff-shapes of Cu nanoparticles with different adsorbates covered. Reprinted with permission from Ref. [53]. Copyright 2018, Springer Nature. Dynamic evolution of the Cu-N bond length with adsorption of one H atom (d) and two H atoms (e). (f) Dynamic evolution of the bond length in the process of Cu atom aggregation. Reprinted with permission from Ref. [153]. Copyright 2022, American Chemical Society.

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The dynamic behaviors of heterogeneous interfaces in electrocatalytic CO₂ reduction

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