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Synergistic interface engineering in Cu-Zn-Ce catalysts for efficient CO2 hydrogenation to methanol

Journal 2025 · IF 17.7 · 发表于 2025 年 9 月 15 日
作者: Yang Chen,Diwen Zhou,Yongli Chang,Hongqiao Lin,Yunzhao Xu,Yong Zhang,Ding Yuan,Lizhi Wu,Yu Tang,Chengyi Dai,Xingang Li,Qinhong Wei,Li Tan
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摘要

CO 2 hydrogenation to CH 3 OH is of great significance for achieving carbon neutrality. Here, we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts (CZC-G) with optimized interfacial synergy, achieving superior performance in CO 2 hydrogenation to methanol. The CZC-G catalyst demonstrated exceptional methanol selectivity (96.8%) and a space-time yield of 73.6 g MeOH ·kg cat –1 ·h –1 under optimized conditions. Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation. Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-O v -Ce ternary interfaces and inhibits the reduction of ZnO, enabling synergistic interactions for efficient CO 2 activation and selective stabilization of formate intermediates (HCOO*), which are critical for methanol synthesis. In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism, while suppressing the reverse water-gas shift reaction. This work underscores the critical role of synthetic methodologies in engineering interfacial structures, offering a strategy for designing high-performance catalysts for sustainable CO 2 resource utilization.

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