Enhanced CO2 Conversion to CO by Silica-Supported Perovskite Oxides at Low Temperatures

被引:100
|
作者
Hare, Bryan. J. [1 ]
Maiti, Debtanu [1 ]
Daza, Yolanda A. [1 ]
Bhethanabotla, Venkat R. [1 ]
Kuhn, John N. [1 ]
机构
[1] Univ S Florida, Dept Chem & Biomol Engn, Tampa, FL 33620 USA
来源
ACS CATALYSIS | 2018年 / 8卷 / 04期
基金
美国国家科学基金会;
关键词
CO2; conversion; heterogeneous catalysis; oxide composites; reverse water gas shift chemical looping; characterization; TOTAL-ENERGY CALCULATIONS; CHEMICAL DIFFUSION; IRON-OXIDE; TRANSPORT; CATALYST; SR; EFFICIENCY; PERMEATION; OXIDATION; METALS;
D O I
10.1021/acscatal.7b03941
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
Repurposing of CO2 to valuable hydrocarbons is crucial for energy security and a balanced carbon cycle. Reverse water gas shift chemical looping (RWGS-CL) is capable of efficient CO2 to CO conversion at a low temperature of,similar to 600 degrees C with unprecedented rates using the La0.75Sr0.25FeO3 (LSF) perovskite-type oxide amalgamated with silica. The LSF/SiO2 composite (25% LSF by mass) promotes a notable extent of oxygen vacancies in the active phase, a key parameter for CO, conversion. In each of eight RWGS-CL cycles, CO generation yields of LSF/SiO2 surpass those of LSF alone by about 200%, producing 2.6 mmol of CO g(isF)(-1) at a peak rate of 0.8 mmol CO g(LsF)(-1) min(-1). This significant improvement is concomitant with a decreased average LSF crystallite size retained at these low thermochemical reaction temperatures. Evidence of this enhancement points to perovskite particle size reduction by silica, lattice strain induced by the support, and curtailed quantities of secondary phases that limit accessibility to active surfaces. In this contribution, an appropriate stable platform for improving earth abundancy in perovskite-based redox materials is demonstrated for industrial scale low-temperature CO2 thermochemical conversion.
引用
收藏
页码:3021 / 3029
页数:17
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