Progress on Tuning the Geometric and Electronic Structure of Precious Metal Catalysts for Hydrogen Peroxide Production via Two-Electron Oxygen Reduction

doi:10.19894/j.issn.1000-0518.230048

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (8): 1063-1076.DOI: 10.19894/j.issn.1000-0518.230048

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Progress on Tuning the Geometric and Electronic Structure of Precious Metal Catalysts for Hydrogen Peroxide Production via Two-Electron Oxygen Reduction

Er-Gui LUO(), Tao TANG, Yi WANG, Jun-Ming ZHANG, Yu-Hong CHANG, Tian-Jun HU, Jian-Feng JIA()

Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science of Shanxi Normal University，Taiyuan 030032，China

Received:2023-03-06 Accepted:2023-06-01 Published:2023-08-01 Online:2023-08-24
Contact: Er-Gui LUO,Jian-Feng JIA
About author:jiajf@dns.sxnu.edu.cn
luogui1991@sxnu.edu.cn；
Supported by:
the National Natural Science Foundation of China(22209102);the Natural Science Foundation of Shanxi Province(20210302124473)

Abstract

Abstract:

Electrochemical synthesis of hydrogen peroxide （H₂O₂） via two-electron oxygen reduction reaction （2e-ORR） is featured with cost effectiveness and environmental friendliness， and enables on-site production of H₂O₂ on demand. One of the key technologies is the development of safe， economical and efficient 2e-ORR catalysts. Here， the research progress in precious-metal-based catalytic materials for the synthesis of H₂O₂via 2e-ORR in recent ten years is reviewed. This review starts with the fundamental mechanism of ORR， pointing out the tuning knobs of reaction pathway on precious-metal surfaces， namely， ^*OOH binding energy and O₂ adsorption mode. The regulating methodologies of geometric structure and electronic structure of precious-metal materials are summarized and exemplified， emphasizing the importance of balanced optimization of catalytic activity and selectivity. We have also briefly introduced the lab-scale methods for performance evaluation of 2e-ORR catalysts. Finally， the challenges and prospects of H₂O₂ synthesis catalyzed by precious metals are discussed， especially the catalyst stability and the objective evaluation of cost. This review is expected to provide a reference for rational design of novel 2e-ORR catalysts.

Key words: Electrochemical synthesis of hydrogen peroxide, Oxygen reduction reaction, Precious metal catalysts, Selectivity

CLC Number:

O646

Er-Gui LUO, Tao TANG, Yi WANG, Jun-Ming ZHANG, Yu-Hong CHANG, Tian-Jun HU, Jian-Feng JIA. Progress on Tuning the Geometric and Electronic Structure of Precious Metal Catalysts for Hydrogen Peroxide Production via Two-Electron Oxygen Reduction[J]. Chinese Journal of Applied Chemistry, 2023, 40(8): 1063-1076.

Figures/Tables 7

Fig.1 （A） Schematic illustration of a fuel cell for the synthesis of H2O2［22］；（B） Schematic illustration of a electrolysis cell for the synthesis of H2O2［23］；（C） Schematic diagram of the mechanisms for 4e-ORR and 2e-ORR［42］；（D） 4e-ORR （blue） and 2e-ORR （green） activity volcano curves［42］；（E） Schematic illustration of three modes of O2 adsorption［43］

Fig.2 （A） RRDE setup and （B） H-type cell［52］

Fig.3 （A） HRTEM image of AuPd alloy and adsorption of O2 on Pd isolated atoms （left） and Pd monolayer （right）［62］；（B） H2O2 selectivity of AuPd alloy catalysts with varied Pd content［62］；（C） Schematic depiction of Pt-Hg alloy［27］；（D） Free-energy diagram for 2e-ORR to H2O2 on several metal surfaces［27］；（E） Polarization curve and corresponding H2O2 yield of Pt-Hg/C catalyst in O2-saturated 0.1 mol/L HClO4［27］；（F） Free-energy diagram for 2e-ORR to H2O2 on AuCu and AD-Pt@AuCu［64］

Fig.4 （A） Schematic diagram of Pt surface modified with calix［4］arene molecules［70］；（B） Polarization curve of CN--adsorbed Pt（111） electrode［67］；（C） ORR activity and ring current of CN--adsorbed Pt（111） electrode under different CN- coverage［67］；（D） The effect of carbon coating on the O2 adsorption mode and ORR pathway on Pt/C catalyst［72］

Fig.5 （A） ORR polarization curves and ring currents of Pt/TiN catalysts［73］；（B） Support effect in Pt SACs［74］；（C） Schematic illustration of the preparation of CuS x -supported Pt SACs （h-Pt1-CuS x ）［75］；（D） ORR performance of h-Pt1-CuS x and control samples［75］；（E） AC-STEM image of Pt/HSC［76］；（F） ORR activity and （G） H2O2 selectivity of Pt/HSC and control samples［76］

Fig.6 （A） Size dependence of H2O2 formation on Pt-based catalysts［83］；（B） H2O2 selectivity on crystalline Pd and amorphous Pd nanoparticles［84］；（C） Optimized structures of active sites in Pd δ+-OCNT catalyst and （D） activity volcano plot based on DFT calculations［53］

Fig.7 Tuning strategies of the geometric and electronic structure of precious metal catalysts for 2e-ORR

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Progress on Tuning the Geometric and Electronic Structure of Precious Metal Catalysts for Hydrogen Peroxide Production via Two-Electron Oxygen Reduction

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