Low-Dimensional Metal-Organic Frameworks with High Activity and Selectivity toward Electrocatalytic Chlorine Evolution Reactions

doi:10.1021/acs.jpcc.2c01593

	Low-Dimensional Metal-Organic Frameworks with High Activity and Selectivity toward Electrocatalytic Chlorine Evolution Reactions
	Liu, Junxian 1; Hinsch, Jack Jon 1; Yin, Huajie 2; Liu, Porun 1; Zhao, Huijun 1; Wang, Yun 1
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2022-04-28
卷号	126
ISSN号	1932-7447
DOI	10.1021/acs.jpcc.2c01593
通讯作者	Wang, Yun(yun.wang@griffith.edu.au)
英文摘要	Chlorine gas plays a paramount role in modern industrial chemistry and is one of the most basic chemicals produced by the electrolysis of brine solution. In the past decades, the dimensionally stable anode (DSA) made of RuO2 is the benchmark catalyst for the chlorine evolution reaction (CER) with high activity. However, the drawbacks of the DSA, such as high cost and inferior selectivity, demand the development of low-cost and efficient electrocatalysts for CER. Herein, three low-dimensional Fe/Co/Ni-dithiolene metal-organic frameworks (MOFs) were systematically investigated using the density functional theory. Our calculation results predict that Ni-based dithiolene MOF can efficiently catalyze the CER with a low thermodynamic overpotential of 0.049 V via the Cl* intermediate. The electronic resonance structure of [Ni2+(L center dot-)(L2-)](-) in the Ni-based dithiolene MOF leads to the electron transfer first from S atoms in ligands to Ni cations to achieve a stable electronic configuration, which leads to the most desirable Ni-Cl interaction strength for CER. Moreover, the selectivity to Cl-2 generation is due to its high thermodynamic overpotential of oxygen evolution reaction. Our findings may, therefore, accelerate CER catalyst discoveries beyond DSAs with the optimized electronic structures.
资助项目	Australian Commonwealth Government ; Pawsey Supercomputing Centre in Perth ; Australian government ; Government of Western Australia
WOS关键词	PLANE-WAVE ; OXYGEN EVOLUTION ; COMPETING CHLORINE ; PERFORMANCE ; REDUCTION ; STABILITY ; SURFACE ; OXIDE ; COHP ; DFT
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000797817500016
资助机构	Australian Commonwealth Government ; Pawsey Supercomputing Centre in Perth ; Australian government ; Government of Western Australia
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/130905]
专题	中国科学院合肥物质科学研究院
通讯作者	Wang, Yun
作者单位	1.Griffith Univ, Sch Environm & Sci, Ctr Catalysis & Clean Energy, Gold Coast, Qld 4222, Australia 2.Chinese Acad Sci, Inst Solid State Phys, Hefei 230031, Peoples R China
推荐引用方式 GB/T 7714	Liu, Junxian,Hinsch, Jack Jon,Yin, Huajie,et al. Low-Dimensional Metal-Organic Frameworks with High Activity and Selectivity toward Electrocatalytic Chlorine Evolution Reactions[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2022,126.
APA	Liu, Junxian,Hinsch, Jack Jon,Yin, Huajie,Liu, Porun,Zhao, Huijun,&Wang, Yun.(2022).Low-Dimensional Metal-Organic Frameworks with High Activity and Selectivity toward Electrocatalytic Chlorine Evolution Reactions.JOURNAL OF PHYSICAL CHEMISTRY C,126.
MLA	Liu, Junxian,et al."Low-Dimensional Metal-Organic Frameworks with High Activity and Selectivity toward Electrocatalytic Chlorine Evolution Reactions".JOURNAL OF PHYSICAL CHEMISTRY C 126(2022).