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Rh promoted In2O3 as a highly active catalyst for CO2 hydrogenation to methanol
Catalysis Science & Technology ( IF 5 ) Pub Date : 2020-10-19 , DOI: 10.1039/d0cy01789b
Nazmul Hasan MD Dostagir 1, 2, 3, 4, 5 , Coogan Thompson 6, 7, 8, 9 , Hirokazu Kobayashi 1, 2, 3, 4 , Ayman M. Karim 6, 7, 8, 9 , Atsushi Fukuoka 1, 2, 3, 4 , Abhijit Shrotri 1, 2, 3, 4
Affiliation  

Synthesis of methanol with high selectivity and productivity through hydrogenation of CO2 is highly attractive. This work uses a Rh doped In2O3 catalyst to achieve a high methanol productivity of 1.0 gMeOH h−1 gcat−1 while maintaining the intrinsic high selectivity of pure In2O3. Rh facilitated the dissociation of H2 leading to creation of oxygen vacancies over the In2O3 surface. In addition, Rh atoms also participated in the activation of CO2 to produce formate species with a low activation barrier as evidenced by DFT calculation. Rh species were atomically dispersed in the In2O3 matrix and were stable during a long term reaction. Under reaction conditions, the surface Rh atoms were reduced and were stabilized by charge transfer from neighbouring In atoms. Our results show that incorporation of atomic Rh species in In2O3 can lead to high methanol productivity by creation of oxygen vacancies as well as Rh centred active sites for CO2 activation.

中文翻译:

Rh促进In2O3成为高活性催化剂,用于CO2加氢成甲醇

通过CO 2的氢化以高选择性和高生产率合成甲醇非常有吸引力。这项工作使用Rh掺杂的In 2 O 3催化剂实现了1.0 g MeOH h -1 g cat -1的高甲醇生产率,同时保持了纯In 2 O 3固有的高选择性。Rh促进了H 2的解离,导致在In 2 O 3表面形成氧空位。此外,Rh原子也参与了CO 2的活化DFT计算表明,这种方法可以生产出具有较低活化障碍的甲酸盐物种。Rh原子原子分散在In 2 O 3基质中,并且在长期反应中稳定。在反应条件下,表面Rh原子被还原并通过相邻In原子的电荷转移而稳定。我们的结果表明,在In 2 O 3中引入原子Rh物种可以通过产生氧空位以及以Rh为中心的CO 2活化活性位而导致高甲醇产率。
更新日期:2020-11-05
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