Light-driven CO2 methanation over Au-grafted Ce0.95Ru0.05O2 solid-solution catalysts with activities approaching the thermodynamic limit

被引：117

作者：

Jiang, Haoyang ^{[1
]}

Wang, Linyu ^{[1
]}

Kaneko, Hiroaki ^{[2
]}

Gu, Rongtian ^{[3
]}

Su, Guangxu ^{[4
]}

Li, Le ^{[1
]}

Zhang, Jin ^{[1
]}

Song, Hucheng ^{[5
]}

Zhu, Feng ^{[1
]}

Yamaguchi, Akira ^{[2
]}

Xu, Jun ^{[5
]}

Liu, Fanxin ^{[4
]}

Miyauchi, Masahiro ^{[2
]}

Ding, Weiping ^{[3
]}

Zhong, Miao ^{[1
]}

机构：

[1] Nanjing Univ, Coll Engn & Appl Sci, Natl Lab Solid State Microstruct, Jiangsu Key Lab Artificial Funct Mat, Nanjing, Peoples R China

[2] Tokyo Inst Technol, Sch Mat & Chem Technol, Tokyo, Japan

[3] Nanjing Univ, Sch Chem & Chem Engn, Nanjing, Peoples R China

[4] Zhejiang Univ Technol, Dept Appl Phys, Hangzhou, Peoples R China

[5] Nanjing Univ, Sch Elect Sci & Engn, Nanjing, Peoples R China

来源：

NATURE CATALYSIS | 2023年 / 6卷 / 06期

基金：

中国国家自然科学基金;

关键词：

CHARGE SEPARATION; GAS PROJECTS; H-2; NANOPARTICLES; CONVERSION; SOLAR; CH4; OXIDATION; ENERGY; POWER;

D O I：

10.1038/s41929-023-00970-z

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Photothermal CO2 methanation offers a clean and sustainable solution to store intermittent renewable energy as synthetic CH4. However, its high reaction temperature and low space-time yield hinder its industrial application. Here we report an Au/Ce0.95Ru0.05O2 solid-solution catalyst exhibiting a remarkable photothermal CO2 methanation activity approaching the thermal catalysis limit under visible-near-infrared light irradiation without external heating. Localized surface-plasmon-induced hot-electron injection created abundant oxygen vacancies near the dispersed ruthenium sites, accelerating CO2 methanation. An approximately 6-to 8-fold increase in the pre-exponential factor was evidenced using Arrhenius plot analysis under visible-near-infrared light irradiation. Using a flow reactor, a photothermal CH4 production rate of 473 mmol g(-1) cat h(-1) was obtained at a gas hourly space velocity of 80, 000 ml g(-1) cat h(-1) with similar to 100% CH4 selectivity, similar to 75% single-pass CO2 conversion and excellent durability. Our study offers insights into plasmonic-steered photochemistry, which may open opportunities for the high-yielding synthesis of carbon-based chemicals using solar energy.

引用

页码：519 / 530

页数：12

共 66 条

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