Strategically Constructing Alkali-Metal Interfacial Bridges to Boost Photocatalytic CO2 Methanation on Supported Ni―Ru Bimetallic Catalysts
文献类型: 外文期刊
作者: Guo, Xiaolei;Wu, Yuqi;Zhou, Shengrong;Shao, Yuhang;Izumi, Yasuo;He, Jinlu;Zhang, Hongwei
作者机构:
关键词: alkali-metal interfacial bridges;bimetallic sites;CO2 methanation;metal-support interactions;photocatalysis
期刊名称: ADVANCED SCIENCE
ISSN:
年卷期: 2025 年
页码:
收录情况: SCIE(2025版) ; ; EI(2025版)
摘要: Efficient photocatalytic conversion of CO2 into CH4 is crucial yet challenging due to the complex multi-electron transfer processes and sluggish intermediate transformation. Herein, an innovative strategy is introduced to dramatically enhance photocatalytic CO2 methanation by constructing interfacial alkali-metal bridges (Na-inter) between Ni and Ru nanoparticles over ZrO2 surface. By selectively introducing and subsequently removing excessive surface Na species, stable interfacial Na species are retained, forming a distinctive Ni-0 & horbar;Ni delta+& horbar;Na-inter & horbar;O & horbar;Ru electronic bridge. Comprehensive structural and electronic characterizations (XRD, TEM, XAFS, XPS, DRIFTS) demonstrate that the interfacial Na bridge significantly improves electronic communication between Ni and Ru, enhances charge separation efficiency, optimizes CO2 adsorption, and lowers activation barriers for key intermediates. As a result, the optimized catalyst (0.2Na & horbar;Ni & horbar;Ru/ZrO2) achieves an exceptionally high CH4 production rate of 1882.7 mu molg(-1)h(-1), approximate to 15-fold that of the Na-free catalyst, with excellent stability and durability. DFT calculations reveal that the Na-inter site effectively stabilizes reactive intermediates, greatly accelerating formate to CO conversion and reshaping the reaction pathway. This work highlights alkali-metal-mediated interfacial engineering as a versatile approach to enhance the synergy in multi-component catalysts, opening a new avenue for advanced photocatalytic CO2 reduction.
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