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Ni–In Synergy in CO2 Hydrogenation to Methanol
ACS Catalysis ( IF 12.9 ) Pub Date : 2021-08-29 , DOI: 10.1021/acscatal.1c03170
Jiadong Zhu 1 , Francesco Cannizzaro 1 , Liang Liu 1 , Hao Zhang 1 , Nikolay Kosinov 1 , Ivo A W Filot 1 , Jabor Rabeah 2 , Angelika Brückner 2 , Emiel J M Hensen 1
Affiliation  

Indium oxide (In2O3) is a promising catalyst for selective CH3OH synthesis from CO2 but displays insufficient activity at low reaction temperatures. By screening a range of promoters (Co, Ni, Cu, and Pd) in combination with In2O3 using flame spray pyrolysis (FSP) synthesis, Ni is identified as the most suitable first-row transition-metal promoter with similar performance as Pd–In2O3. NiO–In2O3 was optimized by varying the Ni/In ratio using FSP. The resulting catalysts including In2O3 and NiO end members have similar high specific surface areas and morphology. The main products of CO2 hydrogenation are CH3OH and CO with CH4 being only observed at high NiO loading (≥75 wt %). The highest CH3OH rate (∼0.25 gMeOH/(gcat h), 250 °C, and 30 bar) is obtained for a NiO loading of 6 wt %. Characterization of the as-prepared catalysts reveals a strong interaction between Ni cations and In2O3 at low NiO loading (≤6 wt %). H2-TPR points to a higher surface density of oxygen vacancy (Ov) due to Ni substitution. X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and electron paramagnetic resonance analysis of the used catalysts suggest that Ni cations can be reduced to Ni as single atoms and very small clusters during CO2 hydrogenation. Supportive density functional theory calculations indicate that Ni promotion of CH3OH synthesis from CO2 is mainly due to low-barrier H2 dissociation on the reduced Ni surface species, facilitating hydrogenation of adsorbed CO2 on Ov.

中文翻译:

镍-铟在 CO2 加氢制甲醇中的协同作用

氧化铟 (In 2 O 3 ) 是一种用于从 CO 2选择性合成CH 3 OH的有前途的催化剂,但在低反应温度下表现出不足的活性。通过使用火焰喷雾热解 (FSP) 合成筛选与 In 2 O 3结合的一系列促进剂(Co、Ni、Cu 和 Pd),Ni 被确定为最合适的第一排过渡金属促进剂,其性能与Pd-In 2 O 3。NiO–In 2 O 3通过使用 FSP 改变 Ni/In 比来优化。所得催化剂包括 In 2 O 3和 NiO 端元具有相似的高比表面积和形貌。CO 2加氢的主要产物是 CH 3 OH 和 CO,其中 CH 4仅在高 NiO 负载量(≥75 wt %)下观察到。最高的 CH 3 OH 速率(~0.25 g MeOH /(g cat h)、250 °C 和 30 bar)是在 NiO 负载量为 6 wt% 时获得的。所制备催化剂的表征表明,在低 NiO 负载量(≤6 wt%)下,Ni 阳离子与 In 2 O 3之间存在强相互作用。H 2 -TPR 指向更高的氧空位表面密度 (O v) 由于 Ni 取代。所用催化剂的 X 射线光电子能谱、X 射线吸收光谱和电子顺磁共振分析表明,在 CO 2氢化过程中,Ni 阳离子可以以单原子和非常小的簇形式还原为 Ni 。支持性密度泛函理论计算表明,Ni 促进从 CO 2合成CH 3 OH主要是由于还原的 Ni 表面物质上的低势垒 H 2解离,促进了 O v上吸附的 CO 2 的氢化。
更新日期:2021-09-17
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