Xuan Xiaoxu, Cheng Jun, Yang Xiao, Zhou Junhu, Cen Kefa
State Key Laboratory of Clean Energy Utilization, Zhejiang University Hangzhou 310027 China
RSC Adv. 2019 Apr 5;9(19):10635-10644. doi: 10.1039/c9ra00176j. eCollection 2019 Apr 3.
Carbon supported nano-metal catalysts are expected to improve CO reduction selectivity and efficiency due to the addition of more active sites and enhancement of electron transport ability. In this study, HKUST-1 was pyrolyzed and decorated with Pt to prepare Pt-Cu/C catalysts. The catalytic effect of the catalysts with different Pt contents in the CO photoeletrochemical reduction reaction (COPRR) were compared. The total carbon atom conversion rate in COPRR experiments using Pt-Cu/C catalysts first increased to a peak when using 1.6 wt% Pt-Cu/C catalyst and then decreased with the increase of Pt content. The 1.6 wt% Pt-Cu/C catalyst showed good hydrogen evolution reaction (HER) inhibiting ability compared with other Pt-Cu/C catalysts. Density functional theory (DFT) calculations were conducted to give an insight into the COPRR mechanism on some possible active sites in Pt-Cu/C catalysts. The result demonstrated that HER was more likely to be inhibited on the Cu/Pt active surface and at the same time COPRR was promoted.
碳负载的纳米金属催化剂有望通过增加更多活性位点和增强电子传输能力来提高CO还原的选择性和效率。在本研究中,对HKUST-1进行热解并用Pt修饰以制备Pt-Cu/C催化剂。比较了不同Pt含量的催化剂在CO光电化学还原反应(COPRR)中的催化效果。在使用Pt-Cu/C催化剂的COPRR实验中,总碳原子转化率在使用1.6 wt% Pt-Cu/C催化剂时先增加到峰值,然后随着Pt含量的增加而降低。与其他Pt-Cu/C催化剂相比,1.6 wt% Pt-Cu/C催化剂表现出良好的析氢反应(HER)抑制能力。进行了密度泛函理论(DFT)计算,以深入了解Pt-Cu/C催化剂中一些可能的活性位点上的COPRR机理。结果表明,在Cu/Pt活性表面上HER更有可能受到抑制,同时COPRR得到促进。