Huang Jialu, Ni Zhiming, Song Xiaofan, Li Han, Chen Xiaolei, Zhang Aichuang, Yang Hu, Liu Yuan, Zhu Peng, Hua Ping, Yuan Xiaolei
School of Chemistry and Chemical Engineering, Nantong University, 9 Seyuan Road, Nantong 226019, China.
Sales Department, Petrochina Tuha Oilfield Company, Shanshan County, Turpan 838200, Xinjiang, China.
ACS Omega. 2022 Sep 28;7(40):35720-35726. doi: 10.1021/acsomega.2c03693. eCollection 2022 Oct 11.
PdPb nanocrystals have drawn considerable attention due to their excellent catalytic properties, while their practical applications have been impeded by the severe degradation of activity, which is caused by the adsorption of intermediates (especially CO) during the operation. Herein, we first present porous PdPb alloys with the incorporation of amorphous Pb(OH) species as highly active and stable electrocatalysts. Alloying Pd with Pb species is initially proposed to optimize the Pd-Pd interatomic distance and adjust the d-band center of Pd. Importantly, the amorphous Pb(OH) species are beneficial to promoting the formation of OH and the removal of CO. Therefore, PdPb-Pb(OH) catalysts show a mass activity of 3.18 A mg and keep excellent stability for the ethanol oxidation reaction (EOR). In addition, further CO stripping and a series of CO poisoning experiments indicate that PdPb-Pb(OH) composites possess much better CO tolerance benefiting from the tuned electronic structure of Pd and surface incorporation of Pb(OH) species.
钯铅纳米晶体因其优异的催化性能而备受关注，但其实际应用却因运行过程中中间体（尤其是一氧化碳）的吸附导致活性严重下降而受阻。在此，我们首次展示了掺入非晶态氢氧化铅物种的多孔钯铅合金作为高活性和稳定的电催化剂。最初提出将钯与铅物种合金化以优化钯-钯原子间距离并调整钯的d带中心。重要的是，非晶态氢氧化铅物种有利于促进羟基的形成和一氧化碳的去除。因此，钯铅-氢氧化铅催化剂显示出3.18 A mg的质量活性，并在乙醇氧化反应（EOR）中保持优异的稳定性。此外，进一步的一氧化碳剥离和一系列一氧化碳中毒实验表明，钯铅-氢氧化铅复合材料由于钯的电子结构调整和表面掺入氢氧化铅物种而具有更好的一氧化碳耐受性。
