Dilute Aqueous-Aprotic Hybrid Electrolyte Enabling a Wide Electrochemical Window through Solvation Structure Engineering

Wu, Shuilin1,2; Su, Bizhe3; Sun, Mingzi4; Gu, Shuai5; Lu, Zhouguang6; Zhang, Kaili5; Yu, Denis Y. W.3; Huang, Bolong4; Wang, Pengfei7,8; Lee, Chun-Sing1,2; Zhang, Wenjun1,2

2021-08-01

10.1002/adma.202102390

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

The application of superconcentrated aqueous electrolytes has shown great potential in developing high-voltage electrochemical double-layer capacitors (EDLCs). However, the broadening of the electrochemical window of such superconcentrated electrolytes is at the expense of their high cost, low ionic conductivity, high density, and narrow operating temperature range. Herein, the electrochemical window of water (>3 V) at low salt concentration (3 m) is expanded by using an aprotic solvent, i.e., trimethyl phosphate (TMP), to regulate the solvation structure of the electrolyte. Benefiting from the low salt concentration, such electrolyte is simultaneously featured with high ionic conductivity, low density, and wide temperature compatibility. Based on the dilute hybrid electrolyte, EDLCs constructed by using porous graphene electrodes are able to operate within an enlarged voltage range of 0-2.4 V at a wide range of temperatures from -20 to 60 degrees C. They also present excellent rate capability and cycle stability, i.e., 83% capacitance retention after 100 000 cycles. Density functional theory calculations verify that TMP induces a significant electronic modulation for the bonding environment of the electrolyte. This enables the stronger binding of Na+-H2O with freely migrating TMP to expand the voltage window to exceed the potential limitation of aqueous electrolytes.

aqueous supercapacitors hybrid electrolytes solvation structures

SCI ; EI

英语

NI论文

其他

General Research Fund[GRF CityU 1307619] ; CityU Applied Research Grant[ARG 9667208] ; National Science Foundation of China[51872249]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000692117300001

WILEY-V C H VERLAG GMBH

20213510845411

Capacitance ; Chemical bonds ; Density functional theory ; Graphite electrodes ; Ionic conductivity ; Solvation

Electricity: Basic Concepts and Phenomena:701.1 ; Electric Batteries and Fuel Cells:702 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Probability Theory:922.1

MATERIALS SCIENCE

Web of Science

1.City Univ Hong Kong, Dept Mat Sci & Engn, 83 Tat Chee Ave, Hong Kong, Peoples R China
2.City Univ Hong Kong, Ctr Super Diamond & Adv Films, 83 Tat Chee Ave, Hong Kong, Peoples R China
3.City Univ Hong Kong, Sch Energy & Environm, 83 Tat Chee Ave, Hong Kong, Peoples R China
4.Hong Kong Polytech Univ, Dept Appl Biol & Chem Technol, Kowloon, Hong Kong, Peoples R China
5.City Univ Hong Kong, Dept Mech Engn, 83 Tat Chee Ave, Hong Kong, Peoples R China
6.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Guangdong Hong Kong Macao Joint Lab Photon Therma, Shenzhen 518055, Guangdong, Peoples R China
7.Chinese Acad Sci, Key Lab Photochem Convers & Optoelect Mat, Beijing 100190, Peoples R China
8.Chinese Acad Sci, CityU CAS Joint Lab Funct Mat & Devices, Beijing 100190, Peoples R China

Wu, Shuilin,Su, Bizhe,Sun, Mingzi,et al. Dilute Aqueous-Aprotic Hybrid Electrolyte Enabling a Wide Electrochemical Window through Solvation Structure Engineering[J]. ADVANCED MATERIALS,2021,33.

Wu, Shuilin.,Su, Bizhe.,Sun, Mingzi.,Gu, Shuai.,Lu, Zhouguang.,...&Zhang, Wenjun.(2021).Dilute Aqueous-Aprotic Hybrid Electrolyte Enabling a Wide Electrochemical Window through Solvation Structure Engineering.ADVANCED MATERIALS,33.

Wu, Shuilin,et al."Dilute Aqueous-Aprotic Hybrid Electrolyte Enabling a Wide Electrochemical Window through Solvation Structure Engineering".ADVANCED MATERIALS 33(2021).