Wang Lingxiang, Fang Wei, Wang Liang, Xiao Feng-Shou
Department of Chemistry, Zhejiang University, Hangzhou, 310028, P. R. China.
Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027, P. R. China.
ChemSusChem. 2020 Dec 7;13(23):6300-6306. doi: 10.1002/cssc.202001784. Epub 2020 Sep 10.
Strong metal-support interactions (SMSI) could improve the performance of nanoparticle catalysts through the electronic and geometric modulation of the reducible metal oxide supports. Here, SMSI is demonstrated to occur for catalysts with non-oxide carrier, such as NbOPO -supported Rh nanoparticles, under reduction treatment at low temperature. During CO hydrogenation, this Rh/NbOPO catalyst with SMSI exhibits impressive CO selectivity at high CO conversion in a wide temperature range with hindered methanation. For example, over 98.9 % CO selectivity was obtained with 39.9 % CO conversion at 500 °C. Mechanism investigations demonstrate that the SMSI results in the formation of a metal-support interface with weaker CO adsorption than the metallic Rh sites, thus accelerating the CO desorption, which hinders deep hydrogenation. Rh nanoparticles with small diameter of about 1.1 nm is sinter-resistant with unchanged performance during a long-period test. This work might extend the investigation of SMSI from oxides to phosphate supports, which helps optimizing the selectivity and stability of metal nanoparticle catalysts.
强金属-载体相互作用（SMSI）可通过对可还原金属氧化物载体进行电子和几何调制来提高纳米颗粒催化剂的性能。在此，已证明在低温还原处理下，对于具有非氧化物载体的催化剂，如负载在NbOPO上的Rh纳米颗粒，会发生SMSI。在CO加氢过程中，这种具有SMSI的Rh/NbOPO催化剂在宽温度范围内、在高CO转化率下且甲烷化受阻时，表现出令人印象深刻的CO选择性。例如，在500°C时，CO转化率为39.9%时，CO选择性超过98.9%。机理研究表明，SMSI导致形成金属-载体界面，该界面上CO的吸附比金属Rh位点弱，从而加速了CO脱附，这阻碍了深度加氢。直径约为1.1 nm的小尺寸Rh纳米颗粒在长期测试中具有抗烧结性能且性能不变。这项工作可能会将SMSI的研究从氧化物扩展到磷酸盐载体，这有助于优化金属纳米颗粒催化剂的选择性和稳定性。
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