Yu Hongbo, Zhao Jihao, Wu Chunzheng, Yan Bo, Zhao Shuangliang, Yin Hongfeng, Zhou Shenghu
Shanghai Key Laboratory of Multiphase Materials Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, P. R. China.
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, 1219 Zhongguan West Road, Ningbo 315201, Zhejiang, P. R. China.
Langmuir. 2021 Feb 9;37(5):1894-1901. doi: 10.1021/acs.langmuir.0c03367. Epub 2021 Jan 25.
Decoration of noble metals with transition-metal oxides has been intensively studied for heterogeneous catalysis. However, controllable syntheses of metal-metal oxide heterostructures are difficult, and elucidation of such interfaces is still challenging. In this work, supported IrCo alloy nanoparticles are transformed into supported Ir-CoO close-contact nanostructures by calcination and following selective reduction. Relative to Ir/AlO, Ir-CoO/AlO shows greatly enhanced activities for the hydrogenation of furfural derivatives to the corresponding furfuryl alcohol derivatives with more than 99% selectivity and demonstrates significantly improved activities and selectivity for hydrogenations of α,β-unsaturated aldehydes to α,β-unsaturated alcohols. The modification of Ir surfaces with CoO prevents Ir nanoparticles from growing, achieving high thermal and catalytic stabilities. Theoretic calculation suggests that the better catalytic performance of Ir-CoO/AlO is ascribed to the Ir-CoO interaction, which promotes the absorption of furfural as well as desorption of furfuryl alcohol, resulting in enhanced catalytic activities.
过渡金属氧化物修饰贵金属已在多相催化领域得到深入研究。然而,金属-金属氧化物异质结构的可控合成具有挑战性,阐释此类界面仍然困难重重。在本工作中,负载型IrCo合金纳米颗粒经煅烧及后续选择性还原转化为负载型Ir-CoO紧密接触纳米结构。相对于Ir/AlO,Ir-CoO/AlO对糠醛衍生物加氢生成相应糠醇衍生物表现出大幅增强的活性,选择性超过99%,并且对α,β-不饱和醛加氢生成α,β-不饱和醇的活性和选择性也显著提高。用CoO修饰Ir表面可防止Ir纳米颗粒生长,实现高热稳定性和催化稳定性。理论计算表明,Ir-CoO/AlO更好的催化性能归因于Ir-CoO相互作用,该相互作用促进了糠醛的吸附以及糠醇的脱附,从而提高了催化活性。