Wang Cong-Xiao, Liu Hao-Xin, Gu Hao, Li Jin-Ying, Lai Xiao-Meng, Fu Xin-Pu, Wang Wei-Wei, Fu Qiang, Wang Feng Ryan, Ma Chao, Jia Chun-Jiang
Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, China.
Department of Chemical Engineering, University College London, Roberts Building, Torrington Place, London, WC1E 7JE, UK.
Nat Commun. 2024 Sep 27;15(1):8290. doi: 10.1038/s41467-024-52547-4.
The reverse water gas shift reaction can be considered as a promising route to mitigate global warming by converting CO into syngas in a large scale, while it is still challenging for non-Cu-based catalysts to break the trade-off between activity and selectivity. Here, the relatively high loading of Ni species is highly dispersed on hydroxylated TiO through the strong Ni and -OH interactions, thereby inducing the formation of rich and stable Ni clusters (~1 nm) on anatase TiO during the reverse water gas shift reaction. This Ni cluster/TiO catalyst shows a simultaneous high CO conversion and high CO selectivity. Comprehensive characterizations and theoretical calculations demonstrate Ni cluster/TiO interfacial sites with strong CO activation capacity and weak CO adsorption are responsible for its unique catalytic performances. This work disentangles the activity-selectivity trade-off of the reverse water gas shift reaction, and emphasizes the importance of metal-OH interactions on surface.
逆水煤气变换反应可被视为一种通过大规模将CO转化为合成气来缓解全球变暖的有前景的途径，而对于非铜基催化剂而言，打破活性与选择性之间的权衡仍然具有挑战性。在此，相对高负载的Ni物种通过强烈的Ni与-OH相互作用高度分散在羟基化的TiO上，从而在逆水煤气变换反应过程中诱导在锐钛矿TiO上形成丰富且稳定的Ni簇（约1纳米）。这种Ni簇/TiO催化剂表现出同时具有高CO转化率和高CO选择性。综合表征和理论计算表明，具有强CO活化能力和弱CO吸附的Ni簇/TiO界面位点是其独特催化性能的原因。这项工作解开了逆水煤气变换反应的活性-选择性权衡问题，并强调了表面上金属-OH相互作用的重要性。
