English

Progress on Entropy Production Engineering for Electrochemical Catalysis

• Xinyi Zhang ^1, ,
• Kai Ren ^1, ,
• Yanning Liu ^1, ,
• Zhenyi Gu ^2, ,
• Zhixiong Huang ^2, ,
• Shuohang Zheng ^2, ,
• Xiaotong Wang ^2, ,
• Jinzhi Guo ^2, ,
• Igor V. Zatovsky ^3, ,
• Junming Cao ^{2, ,} ,
• Xinglong Wu ^{1, 2, ,}

• 1.

  Faculty of Chemistry, Northeast Normal University, Changchun 130024, China

• 2.

  MOE Key Laboratory for UV Light-Emitting Materials and Technology, Northeast Normal University, Changchun 130024, China

• 3.

  F.D. Ovcharenko Institute of Biocolloidal Chemistry, NAS Ukraine, Kyiv 03142, Ukraine

Corresponding author: Email: jmcao@nenu.edu.cn (J.C.); Email: xinglong@nenu.edu.cn (X.W.)

• Received Date: 29 July 2023
  Accepted Date: 03 September 2023
  Revised Date: 31 August 2023
  Available Online: 15 July 2024
• Fund Project:

  the National Key R&D Program of China 

  the National Natural Science Foundation of China 

  the Natural Science Foundation of Jilin Province 

  the 111 Project 

  the China Postdoctoral Science Foundation 

  the China Postdoctoral Science Foundation 

  the Fundamental Research Funds for the Central Universities 

Abstract: As for the accurate synthesis of high-performance electrochemical catalysts with good robustness, the rational design on atomic level is still a priority. Entropy, as one of the most significant thermodynamic parameters, measure the disorder of a system, which is a significant quantity for materials. The values are primarily determined by the crystal structure, magnetic moments and the atomic and electronic vibrations of the materials. According to the configurational entropy of the system, we usually divide the material into low entropy materials (LEMs) (ΔS_mix < 1R), medium entropy materials (MEMs) (1R ≤ ΔS_mix ≥ 1.5R) and high entropy materials (HEMs) (ΔS_mix > 1.5R), where R is the gas molar constant. HEMs are those that consist of five or more major elements of roughly equal proportion, in a highly uniform, random manner, which typically consist of one or two major elements compared to traditional materials. As the entropy value increases, the intrinsic physical, chemical and structural properties of the material change accordingly, resulting in special physicochemical properties (e.g., strength, electrical conductivity, corrosion resistance, etc.). Moreover, due to its multi-element combination, the HEMs can be precisely regulated by selecting different elements and their ratios according to the needs, which overcomes the limitations of the traditional catalysts in terms of relatively single component, structure and field of application. Importantly, the synergistic high entropy effect and multi-component arrangement at the atomic-level interface produced by the coexistence of different metal elements in HEMs can exert higher catalytic activity, selectivity and stability in different reactions. This has attracted a lot of attention from researchers, especially in the field of electrocatalysis. In this review systematically summarizes the fundamental concepts of high-entropy catalysts (HECs), synthetic approaches ("top-down" and "bottom-up"), and the structure-performance relationships of HEMs in different types of electrocatalytic processes, mainly including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), alcohol oxidation reaction (AOR), nitrogen reduction reaction (NRR), and carbon dioxide reduction reaction (CO₂RR) etc. Thus, the advantages and potential of high-performance electrocatalysts based on entropy increase engineering are illuminate. At the same time, it is summarized and discussed that HECs are currently facing problems and challenges such as complicated material rational design, complex preparation process, the mechanism of electrocatalytic processes in which multiple metal elements interact is ambiguous, and poor stability under extreme reaction conditions. Finally, the main problems and challenges facing the current HECs research. We look forward to the future design ideas, synthesis methods different research areas and industrial applications of HECs based on entropy enhancement engineering.

Key words:
• Entropy production
•  /  Synthesis
•  /  Electrochemistry
•  /  High-entropy catalyst
•  /  Electrocatalysis

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