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Synergistic confinement and alloying effects in Pd-based catalysts for efficient and stable CO2reduction 认领 引用
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作者 Yujun Cheng Xi Li +6 位作者 Ziyi Gao Yao Yao Chuan Long Jiasi Zuo Haikun Xu Qi Liu Xiaoqing Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第7期1-11,I0002,共11页
Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limi... Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limiting its catalytic activity and stability.To address this critical bottleneck,this study proposes and implements a synergistic regulation strategy combining alloying and spatial confinement effects.This approach designs a composite catalyst by encapsulating boron-silver co-doped palladium alloy nanoparticles(B-Ag4Pd6)within hollow porous resin carbon spheres(HPRCS).In an H-cell,this catalyst achieved a CO Faradaic efficiency of 96.19%at jCO=24.8 mA/cm2 and maintained stable performance for 80 h.Even under flow cell conditions,it sustained 91.23%CO selectivity at jCO=157.86 mA/cm2 over 60 h.Experimental comparisons confirmed the significant promoting effect of spatial confinement on CO2RR.Furthermore,in situ ATR-FTIR spectroscopy and density functional theory(DFT)calculations reveal that B/Ag alloying downshifts the Pd d-band center,optimizes(*)^COOH and(*)^CO adsorption,and the confined Hmicroenvironment accelerates CO formation while suppressing hydrogen evolution.This study not only successfully addressed the issue of carbon intermediate poisoning on Pd surfaces through alloying and microenvironmental regulation,but also provides novel insights and approaches for designing high-performance CO2RR catalysts that integrate electronic structure control with microenvironmental engineering. 展开更多
关键词 CO2electroreduction Pd‑based alloy catalysts Confinement effect Interfacial microenvironment engineering
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