首页|Practical four-electron zinc-iodine aqueous batteries enabled by orbital hybridization induced adsorption-catalysis

Practical four-electron zinc-iodine aqueous batteries enabled by orbital hybridization induced adsorption-catalysis

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The successive I-/I0/I+redox couples in the four-electron zinc-iodine aqueous battery(4eZIB)is plagued by the instability of the electrophilic I+species,which could either be hydrolyzed or be neutralized by the I3 redox intermediates.We present an adsorption-catalysis approach that effectively suppresses the hydrolysis of ICl species and also provides an enhanced reaction kinetics to surpass the formation of trii-odide ions.We elucidate that the improved stability is attributed to the pronounced orbital hybridization between the d orbitals of Fe-N4 moieties(atomic Fe supported on nitrogen doped carbon)and the p orbi-tals of iodine species(I2 and ICl).Such d-p orbital hybridization leads to enhanced adsorption for iodine species,increased energy barrier for proton detachment from the ICl·HOH intermediate during hydroly-sis,and efficient catalysis of the iodine redox reactions with high conversion efficiency.The proposed 4eZIB demonstrates practical areal capacity(＞3 mAh cm-2)with a near-unity coulombic efficiency,high energy density of 420 Wh kg-1(based on cathode mass),and long-term stability(over 10,000 cycles).Even at-20 ℃,the battery exhibits stable performance for over 1000 cycles with high iodine utilization ratio.

IClTriiodideHydrolysisElectrocatalysisd-p orbital hybridization

Tingting Liu、Chengjun Lei、Huijian Wang、Chen Xu、Wenjiao Ma、Xin He、Xiao Liang

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State Key Laboratory of Chem/Bio-Sensing and Chemometrics,Advanced Catalytic Engineering Research Center of the Ministry of Education,College of Chemistry and Chemical Engineering,Hunan University,Changsha 410082,China

National Key R&D Program of ChinaNational Key R&D Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNatural Science Foundation of Hunan ProvinceMajor Program of the Natural Science Foundation of Hunan Province

2022YFB38077002019YFA021060051972107223090482023JJ401212021JC0006

2024

10.1016/j.scib.2024.02.014

科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN：1001-6538
年,卷(期)：2024.69(11)