光驱动C1转换到高附加值化学品的研究进展

doi:10.7503/cjcu20190641

摘要/Abstract

摘要：

阐述了光驱动C1化学的最新研究进展, 分别对光驱动费托合成、水煤气变换、二氧化碳加氢、甲烷重整和甲醇重整制氢的研究进行了综述, 提出了当前研究存在的问题及发展方向.

关键词: 光驱动催化, C1化学, 高附加值化学品, 费托合成, 二氧化碳加氢

Abstract:

We summarized recent progresses of photo-driven C1 chemistry. Latest researches on photo-driven Fischer-Tropsch synthesis, Water-Gas shift, carbon dioxide hydrogenation, methane reforming, and methanol reforming for hydrogen production were systematically reviewed. In addition, the existing problems as well as prospects were also proposed in the research field.

Key words: Photo-driven catalysis, C1 chemistry, Value-added chemicals, Fischer-Tropsch synthesis, CO₂ hydrogenation

中图分类号:

O643

TrendMD:

李振华, 施润, 赵家琦, 张铁锐. 光驱动C1转换到高附加值化学品的研究进展. 高等学校化学学报, 2020, 41(4): 604.

LI Zhenhua, SHI Run, ZHAO Jiaqi, ZHANG Tierui. Research Progress of Photo-driven C1 Conversion to Value-added Chemicals ^†. Chem. J. Chinese Universities, 2020, 41(4): 604.

图/表 8

Fig.1 Schematic showing the reaction process FTS over Ru/graphene under light irradiation(A) and selectivities of photocatalytic FTS hydrocarbons with or without irradiation at different temperatures(B)[46]Copyright 2015, American Chemical Society.

Fig.2 Potential-energy profile of the most possible reaction paths for syngas conversion on Ni(111) and 4O/Ni(111)(A)[47], fabrication of Co-x catalysts and their light-driven FTS performance(B)[48], the potential energy profile of CO dissociation on Co3O4(220), Co(111)/Co3O4(220), and Co(111), CH2 coupling and C2H4 hydrogenation on Co(111)/Co3O4(220) and Co(111)(C)[48], reductive transformation of ZnFeAl-LDH nanosheets to Fe-x catalysts and their photocatalytic behavior in FTS(D)[49] and energy profiles for CO2 formation, C2H4 adsorption and hydrogenation(E)[49](A) Copyright 2016, Wiley-VCH; (B, C) Copyright 2018, Wiley-VCH; (D, E) Copyright 2018, Wiley-VCH.

Fig.3 Two possible mechanisms to rationalize the differences in the UV-Vis or visible light photocatalytic activity of Au/TiO2(A)[52], temporal profile of CO consumption(a), CO2 evolution(b) and H2 evolution(c) over a Au/TiO2(1%) catalyst under solar light irradiation(B)[52], H2 evolution rates and CO conversion of CuOx/Al2O3-19, CuOx/Al2O3-2, Pt/Al2O3-2 and Au/Al2O3-2 catalysts(C)[53] and cycling measurements of WGS reaction under photothermal condition over CuOx/Al2O3 catalyst(D)[53](A, B) Copyright 2013, Royal Society of Chemistry; (C, D) Copyright 2019, Wiley-VCH.

Fig.5 Reaction mechanism for CO and CH4 evolution on a rhodium nanocube(A)[58], schematic presence of the formation of ultrathin LDH structure with abundant surface hydroxyl groups(B)[60] and photothermal conversion of CO2 and cumulative yield of CH4 over Ru loaded catalysts under different flow rates(F. R. ) of CO2 and H2 mixture(C) [60](C) S1: Ru@FL-LDHs; S2: Ru@LDHs; S3: Ru@SiO2. (A) Copyright 2017,Nature Publishing Group; (B, C) Copyright 2016, Wiley-VCH.

Fig.6 Illustration of the different CoFe-x catalysts formed by hydrogen reduction of CoFeAl-LDH nanosheets at different temperatures and their catalytic activities for CO2 hydrogenation(A), time course of CO2 conversion and product selectivities for CO2 hydrogenation over CoFe-650 under UV-Vis irradiation(B) and the hydrocarbon product distribution obtained over CoFe-650 under UV-Vis irradiation for 2 h(C)[61]Copyright 2018, Wiley-VCH.

Fig.7 Schematic of energy transfer from photoexcited hot carriers to adsorbate states and proposed mechanism for SRM reaction on Rh/TiO2 under visible light illumination(A)[65], a schematic illustration of the solar-light-driven thermocatalytic(B) and the catalytic activity of SCM-Ni/SiO2 for CRM versus reaction time under the focused full-solar-spectrum irradiation from the Xe lamp(C)[66](A) Copyright 2018, American Chemical Society; (B, C) Copyright 2018, Wiley-VCH.

Fig.8 Synthesis and methanol photocatalytic application of single-layer MoS2 nanosheets(A), effects of surfactant, methanol, and photocatalysts on MTH efficiency between three different samples while keeping all other experimental conditions the same(B) and DFT calculations(C)[68](B) Sample 1: 10 mL(ca. 8.2 × 103 mg) pure surfactant; sample 2: 5 mL surfactant and 5 mL methanol; sample 3: 2 mg MoS2 in 10 mL methanol. Copyright 2019, Wiley-VCH.

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