二氧化碳加氢合成甲醇氧化铟及其负载金属催化剂研究进展

doi:10.11949/0438-1157.20221072

摘要/Abstract

摘要：

二氧化碳转化利用技术在“双碳”目标达成方面将发挥重要作用。在各种转化利用反应途径中，因为甲醇可以作为有机合成中间体和液态燃料，二氧化碳加氢合成甲醇受到广泛关注。开发高活性、高选择性催化剂是二氧化碳加氢合成甲醇技术发展的关键。近年来，氧化铟及其负载金属催化剂因其高活性、高甲醇选择性而备受关注。氧化铟与一些金属，如金、银、铂、钯、钌、铑、铱、镍、铼等有强相互作用，不仅可以稳定氧化铟、避免氧化铟过还原，还导致催化剂电子结构、反应途径等发生变化，也使得一些本身不具CO₂加氢合成甲醇活性的金属催化剂变为高活性催化剂。CO₂加氢合成甲醇氧化铟系催化剂是通过理论研究预测后经实验证实发现的。CO₂加氢合成甲醇氧化铟及其负载金属催化剂涵盖单原子催化、团簇及纳米颗粒催化剂，是理论可预测的、难得的模型催化剂体系。相关反应途径可用于解释“催化剂”定义。CO₂加氢合成甲醇氧化铟及其负载金属催化剂研究在基础研究和应用两方面都具有重要意义。

关键词: 氧化铟, 催化剂, 二氧化碳, 加氢, 甲醇

Abstract:

The conversion and utilization of carbon dioxide plays important roles in carbon neutrality. Among various options for CO₂ utilization, hydrogenation of CO₂ to methanol attracts increasing attentions because methanol is an important chemical intermediate and also excellent alternative liquid fuel. A highly active catalyst with high methanol selectivity is the key for the potential application of CO₂ hydrogenation to methanol. With their high activity and high methanol selectivity, In₂O₃ and In₂O₃ supported metal catalysts have recently received broad interests. In₂O₃ has strong interaction with metal like gold, silver, platinum, palladium, ruthenium, rhodium, iridium, nickel and rhenium. The strong metal-In₂O₃ interaction can not only stabilize indium oxide, avoid over-reduction of indium oxide, but also lead to the catalyst electronic structure changes, tuning the catalyst to be highly active for selective hydrogenation of CO₂ to methanol. In₂O₃ for CO₂ hydrogenation to methanol was found by the density functional theoretical study. Thus, In₂O₃ and the supported metal catalysts for CO₂ hydrogenation are theoretically predictable and excellent model catalysts for studies of single atom catalyst, cluster and nanoparticle catalysts. The conversion route of the In₂O₃ and its supported catalysts is excellent for the definition of catalyst. These catalysts are important for fundamental studies and also for future applications.

Key words: indium oxide, catalyst, carbon dioxide, hydrogenation, methanol

中图分类号:

TQ 21

沈辰阳, 孙楷航, 张月萍, 刘昌俊. 二氧化碳加氢合成甲醇氧化铟及其负载金属催化剂研究进展[J]. 化工学报, 2023, 74(1): 145-156.

Chenyang SHEN, Kaihang SUN, Yueping ZHANG, Changjun LIU. Research progresses on In₂O₃ and In₂O₃ supported metal catalysts for CO₂ hydrogenation to methanol[J]. CIESC Journal, 2023, 74(1): 145-156.

图/表 7

图1 In2O3(110)表面上CO2加氢合成甲醇的机理[8]

Fig.1 Mechanism of CO2 hydrogenation to methanol over In2O3(110) surface[8]

图2 CO2加氢制甲醇In2O3催化剂的结构演化和动力学[15]

Fig.2 Structural evolution and dynamics of In2O3 catalyst for CO2 hydrogenation to methanol[15]

图3 c-In2O3和h-In2O3表面CO2加氢最优反应途径图示[16]

Fig.3 Schematic illustration of the most favorable CO2 hydrogenation pathways on c-In2O3 and h-In2O3 surfaces[16]

图4 氧化铟负载镍催化剂上CO2加氢合成甲醇的反应途径[19]

Fig.4 The reaction network of CO2 hydrogenation over the In2O3 supported nickel catalysts[19]

图5 Au/In2O3催化剂在CO2加氢反应条件下的AP-XPS图谱[23]

Fig.5 AP-XPS spectra collected under CO2 hydrogenation reaction conditions over Au/In2O3 catalyst [23]

图6 火焰喷雾合成氧化铟负载金属催化剂（载量均为0.5%，质量分数）与氧化铟催化剂CO2加氢活性对比[34]（图中甲醇时空收率以彩色柱状表示、甲醇选择性以米色表示，反应条件：5 MPa, 280℃, H2/CO2 = 4, GHSV = 24000 cm3·(g cat)-1·h-1）

Fig.6 Methanol space-time yield (STY, colored bars) and selectivity (SMeOH, beige bars) during CO2 hydrogenation over undoped In2O3 and M-In2O3 catalysts (0.5%(mass) of metal) prepared by FSP[34] (the methanol STY is assessed at GHSV = 24000 cm3·(g cat)-1·h-1,while SMeOH at constant CO2 conversion (≈3%) and variable WHSV, averaged values measured over 24 h on stream are presented with their corresponding error bars, reaction conditions: T = 280℃, P = 5 MPa, and H2/CO2 = 4)

图7 Re/In2O3催化剂CO2加氢活性测试结果[36](a) 铼的负载量对甲醇时空收率的影响; (b) In2O3, 1Re/In2O3 (铼负载量为1%(质量)催化剂)以及5Re/In2O3(铼负载量为5%(质量)催化剂)在CO2加氢过程中CO2转化率以及产物选择性的对比;(c) 1Re/In2O3催化剂的稳定性测试结果(测试条件:5 MPa, 300℃, H2/CO2 = 4, GHSV = 21000 cm3·(g cat-1)·h-1)

Fig.7 Catalytic performance of Re/In2O3 during CO2 hydrogenation[36](a) effect of Re loadings on the methanol STY; (b) comparison of selectivity and CO2 conversion in the CO2 hydrogenation over In2O3, 1Re/In2O3 and 5Re/In2O3 catalysts; (c) stability test of 1Re/In2O3 for 50 h on stream (reaction conditions: 5 MPa, 300℃, H2/CO2 = 4, GHSV = 21000 cm3·(g cat)-1·h-1)

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