School of Chemistry and Chemical Engineering, Key Laboratory of Functional Inorganic Material Chemistry of Anhui Province, Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei 230601, China.
School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P. R. China.
Inorg Chem. 2023 Mar 27;62(12):5032-5039. doi: 10.1021/acs.inorgchem.3c00293. Epub 2023 Mar 15.
Developing efficient atomic-scale metal-supported catalysts is of great significance for energy conversion technologies. However, the precise modulation of electron transfer between the metal and supporter in atomic-scale metal-supported catalysts to further improve the catalytic activity is still a major challenge. Herein, we show tunable electron transfer between atomic-scale Pt and tungsten nitride/oxide supports (namely, Pt/WN and Pt/WO). Pt/WN with modest electron exchange and Pt/WO with aggressive electron exchange exhibit notably different catalytic activities for the alkaline hydrogen oxidation reaction (HOR), in which Pt/WN shows a 5.7-fold enhancement in HOR intrinsic catalytic performance in comparison to Pt/WO. Additionally, the tunable electronic transfer at the interface of Pt/WN and Pt/WO, as proven by the theoretical calculation, resulted in the discrepancy of the adsorption free energy of the reaction intermediates, as well as catalytic activity, for the HOR process. Our work provides new insights into the design of advanced atomic-scale metal-supported catalysts for electrocatalysis.
开发高效的原子级金属负载催化剂对于能源转换技术具有重要意义。然而，精确调节原子级金属负载催化剂中金属和载体之间的电子转移，以进一步提高催化活性仍然是一个主要挑战。在此，我们展示了原子级 Pt 与氮化钨/氧化钨载体（即 Pt/WN 和 Pt/WO）之间可调变的电子转移。Pt/WN 表现出适度的电子交换，而 Pt/WO 表现出剧烈的电子交换，对碱性氢氧化反应（HOR）表现出明显不同的催化活性，其中 Pt/WN 相对于 Pt/WO 表现出 HOR 本征催化性能提高了 5.7 倍。此外，通过理论计算证明了 Pt/WN 和 Pt/WO 界面可调变的电子转移导致反应中间体的吸附自由能以及 HOR 过程的催化活性存在差异。我们的工作为电催化中先进的原子级金属负载催化剂的设计提供了新的见解。
