Wan Xueying, Li Yifan, Chen Yihong, Ma Jun, Liu Ying-Ao, Zhao En-Dian, Gu Yadi, Zhao Yilin, Cui Yi, Li Rongtan, Liu Dong, Long Ran, Liew Kim Meow, Xiong Yujie
Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovative Center of Chemistry for Energy Materials (iChEM), Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, School of Nuclear Science and Technology, University of Science and Technology of China, Hefei, 230026, Anhui, China.
Sustainable Energy and Environmental Materials Innovation Center, Nano Science and Technology Institute, Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou, 215123, China.
Nat Commun. 2024 Feb 10;15(1):1273. doi: 10.1038/s41467-024-45516-4.
The meticulous design of active sites and light absorbers holds the key to the development of high-performance photothermal catalysts for CO hydrogenation. Here, we report a nonmetallic plasmonic catalyst of MoN/MoO-x nanosheets by integrating a localized surface plasmon resonance effect with two distinct types of active sites for CO hydrogenation. Leveraging the synergism of dual active sites, H and CO molecules can be simultaneously adsorbed and activated on N atom and O vacancy, respectively. Meanwhile, the plasmonic effect of this noble-metal-free catalyst signifies its promising ability to convert photon energy into localized heat. Consequently, MoN/MoO-x nanosheets exhibit remarkable photothermal catalytic performance in reverse water-gas shift reaction. Under continuous full-spectrum light irradiation (3 W·cm) for a duration of 168 h, the nanosheets achieve a CO yield rate of 355 mmol·gcat·h in a flow reactor with a selectivity exceeding 99%. This work offers valuable insights into the precise design of noble-metal-free active sites and the development of plasmonic catalysts for reducing carbon footprints.
活性位点和光吸收体的精心设计是开发用于CO加氢的高性能光热催化剂的关键。在此，我们通过将局域表面等离子体共振效应与两种不同类型的用于CO加氢的活性位点相结合，报道了一种MoN/MoO-x纳米片的非金属等离子体催化剂。利用双活性位点的协同作用，H和CO分子可分别同时吸附并活化在N原子和氧空位上。同时，这种无贵金属催化剂的等离子体效应表明其具有将光子能量转化为局部热量的潜力。因此，MoN/MoO-x纳米片在逆水煤气变换反应中表现出卓越的光热催化性能。在连续全光谱光照射（3 W·cm）168小时的条件下，该纳米片在流动反应器中实现了355 mmol·gcat·h的CO产率，选择性超过99%。这项工作为无贵金属活性位点的精确设计以及用于减少碳足迹的等离子体催化剂的开发提供了有价值的见解。
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