A Universal Additive Design Strategy to Modulate Solvation Structure and Hydrogen Bond Network toward Highly Reversible Fe Anode for Low-Temperature All-Iron Flow Batteries

doi:10.1002/smll.202307354

IMR OpenIR

	A Universal Additive Design Strategy to Modulate Solvation Structure and Hydrogen Bond Network toward Highly Reversible Fe Anode for Low-Temperature All-Iron Flow Batteries
	Yang, Jing 1,2; Yan, Hui 1,2; Zhang, Qi-an 1; Song, Yuanfang 1,2; Li, Ying 1; Tang, Ao 1
通讯作者	Li, Ying(liying@imr.ac.cn) ; Tang, Ao(a.tang@imr.ac.cn)
	2023-10-11
发表期刊	SMALL
ISSN	1613-6810
页码	12
摘要	Aqueous all-iron redox flow batteries (RFBs) are promising competitors for next-generation grid-scale energy storage applications. However, the high-performance operation of all-iron RFBs in a wider temperature range is greatly hindered by inferior iron plating/stripping reaction and low solid-liquid transition temperature at Fe anode. Herein, a universal electrolyte additive design strategy for all-iron RFBs is reported, which realizes a highly reversible and dendrite-free Fe anode at low temperatures. Quantum chemistry calculations first screen several organic molecules with oxygen-containing functional groups and identify N,N-Dimethylacetmide (DMAc) as a potential candidate with low cost, high solubility, and strong interactions with Fe2+ and H2O. Combined experimental characterizations and theoretical calculations subsequently demonstrate that adding DMAc into the FeCl2 solution effectively reshapes the primary solvation shell of Fe2+ via the Fe2+-O (DMAc) bond and breaks hydrogen-bonding network of water through intensified H-bond interaction between DMAc and H2O, thereby affording the Fe anode with enhanced Fe/Fe2+ reversibility and lower freezing point. Consequently, the assembled all-iron RFB achieves an excellent combination of high power density (25 mW cm-2), long charge-discharge cycling stability (95.59% capacity retention in 103 h), and preeminent battery efficiency at -20 degrees C (95% coulombic efficiency), which promise a future for wider temperature range operation of all-iron RFBs. A universal additive design strategy is proposed for all-iron flow batteries at low-temperature operation. By reshaping the solvation structure and breaking hydrogen-bonding network of water, N,N-Dimethylacetmide (DMAc) proves to realize both enhanced Fe/Fe2+ reversibility and lower freezing point, which enables the all-iron flow cell an excellent combination of high power density, long cycling stability and preeminent battery efficiency at -20 degrees C.image
关键词	additive design Fe anodes hydrogen-bond interaction low temperatures solvation structures
资助者	This work was supported by the Natural Science Foundation of Liaoning Province (Grant No. 2023-MS-021). ; Natural Science Foundation of Liaoning Province
DOI	10.1002/smll.202307354
收录类别	SCI
语种	英语
资助项目	This work was supported by the Natural Science Foundation of Liaoning Province (Grant No. 2023-MS-021).[2023-MS-021] ; Natural Science Foundation of Liaoning Province
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001079002200001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：2[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/179419
专题	中国科学院金属研究所
通讯作者	Li, Ying; Tang, Ao
作者单位	1.Chinese Acad Sci, Inst Met Res, Shenyang 110000, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110000, Peoples R China
推荐引用方式 GB/T 7714	Yang, Jing,Yan, Hui,Zhang, Qi-an,et al. A Universal Additive Design Strategy to Modulate Solvation Structure and Hydrogen Bond Network toward Highly Reversible Fe Anode for Low-Temperature All-Iron Flow Batteries[J]. SMALL,2023:12.
APA	Yang, Jing,Yan, Hui,Zhang, Qi-an,Song, Yuanfang,Li, Ying,&Tang, Ao.(2023).A Universal Additive Design Strategy to Modulate Solvation Structure and Hydrogen Bond Network toward Highly Reversible Fe Anode for Low-Temperature All-Iron Flow Batteries.SMALL,12.
MLA	Yang, Jing,et al."A Universal Additive Design Strategy to Modulate Solvation Structure and Hydrogen Bond Network toward Highly Reversible Fe Anode for Low-Temperature All-Iron Flow Batteries".SMALL (2023):12.