文献类型：期刊文献

英文题名：Restructuring the interfacial active sites to generalize the volcano curves for platinum-cobalt synergistic catalysis

作者：Chen, Wenyao[1];Shi, Yao[1];Liu, Changwei[1];Ren, Zhouhong[2];Huang, Zikun[1];Chen, Zhou[1];Zhang, Xiangxue[1];Liang, Shanshan[1];Xie, Lei[3];Lian, Cheng[1];Qian, Gang[1];Zhang, Jing[1];Liu, Xi[2];Chen, De[4];Zhou, Xinggui[1];Yuan, Weikang[1];Duan, Xuezhi[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai, Peoples R China;[2]Shanghai Jiao Tong Univ, In Situ Ctr Phys Sci, Sch Chem & Chem Engn, Shanghai, Peoples R China;[3]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facial, Shanghai, Peoples R China;[4]Norwegian Univ Sci & Technol, Dept Chem Engn, Trondheim, Norway

年份：2024

卷号：15

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001339143700002)】；

基金：This work was financially supported by the National Key R&D Program of China (2021YFA1501403), the Natural Science Foundation of China (22038003, 22178100, 22178101, and U22B20141), the Shanghai Pilot Program for Basic Research (22TQ1400100-15), the Innovation Program of Shanghai Municipal Education Commission, the Program of Shanghai Academic/Technology Research Leader (21XD1421000), the Shanghai Science and Technology Innovation Action Plan (22JC1403800). The authors thank the staff members from the BL11B and BL20U beamline of Shanghai Synchrotron Radiation Facility (SSRF) for assistance during data collection.

语种：英文

摘要：Computationally derived volcano curve has become the gold standard in catalysis, whose practical application usually relies on empirical interpretations of composition or size effects by the identical active site assumption. Here, we present a proof-of-concept study on disclosing both the support- and adsorbate-induced restructuring of Pt-Co bimetallic catalysts, and the related interplays among different interfacial sites to propose the synergy-dependent volcano curves. Multiple characterizations, isotopic kinetic investigations, and multiscale simulations unravel that the progressive incorporation of Co into Pt catalysts, driven by strong Pt-C bonding (metal-support interfaces) and Co-O bonding (metal-adsorbate interfaces), initiates the formation of Pt-rich alloys accompanied by isolated Co species, then Co segregation to epitaxial CoOx overlayers and adjacent Co3O4 clusters, and ultimately structural collapse into amorphous alloys. Accordingly, three distinct synergies, involving lattice oxygen redox from Pt-Co alloy/Co3O4 clusters, dual-active sites engineering via Pt-rich alloy/CoOx overlayer, and electron coupling within exposed alloy, are identified and quantified for CO oxidation (gas-phase), ammonia borane hydrolysis (liquid-phase), and hydrogen evolution reaction (electrocatalysis), respectively. The resultant synergy-dependent volcano curves represent an advancement over traditional composition-/size-dependent ones, serving as a bridge between theoretical models and experimental observations in bimetallic catalysis. Volcano curves have become the gold standard in catalyst design. Here, the authors propose synergy-dependent volcano curves by disclosing both support- and adsorbate-induced catalyst restructuring, ideally bridging the gap between theoretical models and experimental observations.