Sr- and Co-doped LaGaO3-delta with high O-2 and H-2 yields in solar thermochemical water splitting

doi:10.1039/c8ta11957k

	Sr- and Co-doped LaGaO3-delta with high O-2 and H-2 yields in solar thermochemical water splitting
	Li, Can 1; Jiang, Zongxuan 1; Chen, Zhenpan 1,2; Jiang, Qingqing 1; Cheng, Feng 1; Tong, Jinhui 1; Yang, Min 1
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2019-03-21
卷号	7 期号:11 页码:6099-6112
ISSN号	2050-7488
DOI	10.1039/c8ta11957k
通讯作者	Li, Can(canli@dicp.ac.cn)
英文摘要	Solar thermochemical CO2/H2O splitting cycles based on redox oxides have emerged as a potential strategy to store dilute and intermittent solar energy. It is desirable to explore other materials that can convert solar energy into chemical energy with high efficiency. Herein, a thermochemical water splitting (TCWS) cycle based on Sr- and Co-doped LaGaO3-delta (La1-xSrxGa1-yCoyO3-delta) was successfully developed. Compared with inert LaGaO3-, the oxygen vacancy concentration () is gradually increased as the contents of Sr- and/or Co-dopants increased. The value of LaGa0.4Co0.6O3-delta (LGC60) reaches 0.16 after reduction for 40 min at 1350 degrees C, which is 5 and 4 times that of Ce0.85Zr0.15O2-delta and LSMA6464, respectively. The H-2 yield of LGC60 (478 mol H-2 g(perovskite)(-1)) is 15 times that of the current state-of-the-art material, CeO2-delta (32 mol H-2 g(material)(-1)), when reduced at 1350 degrees C and re-oxidized at optimized 800 or 1000 degrees C. 1.0 atom% IrOx as a catalyst doped into the structure of LGC50, named LGC50-Ir(1.0), can increase the H-2 release rate by 1.3-fold. XPS results reveal that the H2O splitting reaction is driven by the Co2+/Co3+ redox pair. DFT calculations predict that the oxygen vacancy formation energies (E-V) of La1-xSrxGa1-yCoyO3 span from nearly 0.7 to about 5.3 eV under vacuum conditions at 1623 K, depending on the contents of Sr- and Co-dopants. Thus, doping Co at the B-site is responsible for the introduction of redox activity, and adjusting Sr- and Co-contents is effective in tuning the and E-V values of La1-xSrxGa1-yCoyO3-delta. It should be pointed out that, at present, the steam to hydrogen conversion ratios for LaGa1- yCoyO3-delta under the used evaluation conditions are still very low (<1%) and far away from the practical demand, which is a common tradeoff in this field, and more attention should be paid in future material screening work. This discovery provides a useful strategy to design perovskite oxides with enhanced TCWS activity and it will promote the development of solar thermochemical fuel conversion science.
资助项目	National Natural Science Foundation of China[21373210] ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences[XDA07040400] ; DICP Fundamental Research Program for Clean Energy[DICP M201302]
WOS关键词	TOTAL-ENERGY CALCULATIONS ; EQUAL-TO X ; HYDROGEN-PRODUCTION ; PEROVSKITE OXIDES ; SOLID-SOLUTIONS ; REDOX ; CYCLE ; FUEL ; MN ; RAMAN
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000463970400018
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; DICP Fundamental Research Program for Clean Energy ; DICP Fundamental Research Program for Clean Energy ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; DICP Fundamental Research Program for Clean Energy ; DICP Fundamental Research Program for Clean Energy ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; DICP Fundamental Research Program for Clean Energy ; DICP Fundamental Research Program for Clean Energy ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; Special Fund for Strategic Pilot Technology of Chinese Academy of Sciences ; DICP Fundamental Research Program for Clean Energy ; DICP Fundamental Research Program for Clean Energy
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/165652]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Li, Can
作者单位	1.Chinese Acad Sci, Dalian Natl Lab Clean Energy, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Li, Can,Jiang, Zongxuan,Chen, Zhenpan,et al. Sr- and Co-doped LaGaO3-delta with high O-2 and H-2 yields in solar thermochemical water splitting[J]. JOURNAL OF MATERIALS CHEMISTRY A,2019,7(11):6099-6112.
APA	Li, Can.,Jiang, Zongxuan.,Chen, Zhenpan.,Jiang, Qingqing.,Cheng, Feng.,...&Yang, Min.(2019).Sr- and Co-doped LaGaO3-delta with high O-2 and H-2 yields in solar thermochemical water splitting.JOURNAL OF MATERIALS CHEMISTRY A,7(11),6099-6112.
MLA	Li, Can,et al."Sr- and Co-doped LaGaO3-delta with high O-2 and H-2 yields in solar thermochemical water splitting".JOURNAL OF MATERIALS CHEMISTRY A 7.11(2019):6099-6112.