Dai Sheng, Huang Tzu-Hsi, Chien Po-Cheng, Lin Cheng-An, Liu Chen-Wei, Lee Sheng-Wei, Wang Jeng-Han, Wang Kuan-Wen, Pan Xiaoqing
Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Institute of Fine Chemicals, School of Chemistry & Molecular Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China.
Department of Materials Science and Engineering, University of California, Irvine, Irvine, California 92697, United States.
J Phys Chem Lett. 2020 Apr 16;11(8):2846-2853. doi: 10.1021/acs.jpclett.0c00213. Epub 2020 Mar 27.
Pt-oxygen-containing species (Pt-OCS) catalysts, in which OCS (e.g., metal-oxides) are decorated on a Pt surface, possess enhanced ethanol oxidation reaction (EOR) activity and stability compared with pure Pt and are promising in practical applications of direct ethanol fuel cells. We investigate the promotion roles of Pt-OCS electrocatalysts toward the EOR via a combination of density functional theory (DFT) calculations and experiments, providing a rational design strategy for Pt-OCS catalysts. It is revealed that Pt-AuO and Pt-SnO excel in EOR activity and stability, respectively, among the DFT screening of various Pt-OCS systems, and this is confirmed by the following experiments. Moreover, an optimized Pt-AuSnO catalyst is proposed by DFT calculations, taking advantage of both Pt-AuO and Pt-SnO. The as-prepared Pt-AuSnO catalyst delivers an EOR activity that is 9.7 times higher than that of Pt and shows desired stability. These findings are expected to elucidate the mechanistic insights into Pt-OCS materials and lead to advanced EOR electrocatalysts.
含铂氧物种（Pt-OCS）催化剂是将氧物种（如金属氧化物）修饰在铂表面，与纯铂相比，具有增强的乙醇氧化反应（EOR）活性和稳定性，在直接乙醇燃料电池的实际应用中具有广阔前景。我们通过密度泛函理论（DFT）计算和实验相结合的方法，研究了Pt-OCS电催化剂对EOR的促进作用，为Pt-OCS催化剂提供了合理的设计策略。研究发现，在各种Pt-OCS体系的DFT筛选中，Pt-AuO和Pt-SnO分别在EOR活性和稳定性方面表现出色，这一点得到了后续实验的证实。此外，通过DFT计算，利用Pt-AuO和Pt-SnO的优势，提出了一种优化的Pt-AuSnO催化剂。所制备的Pt-AuSnO催化剂的EOR活性比Pt高9.7倍，并表现出理想的稳定性。这些发现有望阐明Pt-OCS材料的机理见解，并催生先进的EOR电催化剂。
