文献类型：期刊文献

英文题名：Construction of Ni/In2O3 Integrated Nanocatalysts Based on MIL-68(In) Precursors for Efficient CO2 Hydrogenation to Methanol

作者：Wu, Yiling[1,2] Xu, Kaiji[1,2] Tian, Jian[1,2] Shang, Longmei[1,2] Tan, Kok Bing[1,2] Sun, Hao[3] Sun, Kang[1,2,3] Rao, Xiaoping[1,2] Zhan, Guowu[1,2]

第一作者：Wu, Yiling

机构：[1] Academy of Advanced Carbon Conversion Technology, College of Chemical Engineering, Huaqiao University, 668 Jimei Avenue, Fujian, Xiamen, 361021, China; [2] Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, 668 Jimei Avenue, Fujian, Xiamen, 361021, China; [3] Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry [CAF], 16 Suojin Five Village, Jiangsu, Nanjing, 210042, China

年份：2023

外文期刊名：ACS Applied Materials and Interfaces

收录：EI(收录号：20241315803331)

语种：英文

外文关键词：Binary alloys - Carbon dioxide - Density functional theory - Durability - Fossil fuels - Fourier transform infrared spectroscopy - Indium compounds - Metal nanoparticles - Methanol - Nanocatalysts - Nickel alloys - Nickel compounds - Organometallics - Sintering

摘要：The efficient and economic conversion of CO2 and renewable H2 into methanol has received intensive attention due to growing concern for anthropogenic CO2 emissions, particularly from fossil fuel combustion. Herein, we have developed a novel method for preparing Ni/In2O3 nanocatalysts by using porous MIL-68(In) and nickel(II) acetylacetonate (Ni(acac)2) as the dual precursors of In2O3 and Ni components, respectively. Combined with in-depth characterization analysis, it was revealed that the utilization of MIL-68(In) as precursors favored the good distribution of Ni nanoparticles (～6.2 nm) on the porous In2O3 support and inhibited the metal sintering at high temperatures. The varied catalyst fabrication parameters were explored, indicating that the designed Ni/In2O3 catalyst (Ni content of 5 wt %) exhibited better catalytic performance than the compared catalyst prepared using In(OH)3 as a precursor of In2O3. The obtained Ni/In2O3 catalyst also showed excellent durability in long-term tests (120 h). However, a high Ni loading (31 wt %) would result in the formation of the Ni-In alloy phase during the CO2 hydrogenation which favored CO formation with selectivity as high as 69%. This phenomenon is more obvious if Ni and In2O3 had a strong interaction, depending on the catalyst fabrication methods. In addition, with the aid of in situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory (DFT) calculations, the Ni/In2O3 catalyst predominantly follows the formate pathway in the CO2 hydrogenation to methanol, with HCOO* and *H3CO as the major intermediates, while the small size of Ni particles is beneficial to the formation of formate species based on DFT calculation. This study suggests that the Ni/In2O3 nanocatalyst fabricated using metal-organic frameworks as precursors can effectively promote CO2 thermal hydrogenation to methanol. ? 2024 American Chemical Society.