Zhang An, Liang Yongxiang, Zhang Han, Geng Zhigang, Zeng Jie
Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
Chem Soc Rev. 2021 Sep 7;50(17):9817-9844. doi: 10.1039/d1cs00330e. Epub 2021 Jul 26.
In electrocatalysis, doping regulation has been considered as an effective method to modulate the active sites of catalysts, providing a powerful means for creating a large variety of highly efficient catalysts for various reactions. Of particular interest, there has been growing research concerning the doping of two-dimensional transition-metal compounds (TMCs) to optimize their electrocatalytic performance. Despite the previous achievements, mechanistic insights of doping regulation in TMCs for electrocatalysis are still lacking. Herein, we provide a systematic overview of doping regulation in TMCs in terms of background, preparation, impacts on physicochemical properties, and typical applications including the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, CO reduction reaction, and N reduction reaction. Notably, we bridge the understanding between the doping regulation of catalysts and their catalytic activities via focusing on the physicochemical properties of catalysts from the aspects of vacancy concentrations, phase transformation, surface wettability, electrical conductivity, electronic band structure, local charge distribution, tunable adsorption strength, and multiple adsorption configurations. We also discuss the existing challenges and future perspectives in this promising field.
在电催化中，掺杂调控被认为是调节催化剂活性位点的有效方法，为制备用于各种反应的多种高效催化剂提供了有力手段。特别值得关注的是，关于二维过渡金属化合物（TMCs）的掺杂以优化其电催化性能的研究越来越多。尽管取得了先前的成果，但对于TMCs在电催化中掺杂调控的机理认识仍然不足。在此，我们从背景、制备、对物理化学性质的影响以及典型应用（包括析氢反应、析氧反应、氧还原反应、CO还原反应和N还原反应）等方面对TMCs中的掺杂调控进行了系统综述。值得注意的是，我们通过从空位浓度、相变、表面润湿性、电导率、电子能带结构、局部电荷分布、可调吸附强度和多种吸附构型等方面关注催化剂的物理化学性质，架起了催化剂掺杂调控与其催化活性之间的理解桥梁。我们还讨论了这一充满前景的领域中现有的挑战和未来展望。
