Universal Formation of Single Atoms from Molten Salt for Facilitating Selective CO₂ Reduction

Hao, Qi1,2; Zhen, Cheng3,4; Tang, Qi5,6; Wang, Jiazhi7; Ma, Peiyu8; Wu, Junxiu9; Wang, Tianyang2; Liu, Dongxue10,11; Xie, Linxuan2; Liu, Xiao2; Gu, M. Danny4; Hoffmann, Michael R.12; Yu, Gang13; Liu, Kai2; Lu, Jun9

2024-06-01

10.1002/adma.202406380

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

Clarifying the formation mechanism of single-atom sites guides the design of emerging single-atom catalysts (SACs) and facilitates the identification of the active sites at atomic scale. Herein, a molten-salt atomization strategy is developed for synthesizing zinc (Zn) SACs with temperature universality from 400 to 1000/1100 degrees C and an evolved coordination from Zn-N2Cl2 to Zn-N-4. The electrochemical tests and in situ attenuated total reflectance-surface-enhanced infrared absorption spectroscopy confirm that the Zn-N-4 atomic sites are active for electrochemical carbon dioxide (CO2) conversion to carbon monoxide (CO). In a strongly acidic medium (0.2 m K2SO4, pH = 1), the Zn SAC formed at 1000 degrees C (Zn1NC) containing Zn-N-4 sites enables highly selective CO2 electroreduction to CO, with nearly 100% selectivity toward CO product in a wide current density range of 100-600 mA cm(-2). During a 50 h continuous electrolysis at the industrial current density of 200 mA cm(-2), Zn1NC achieves Faradaic efficiencies greater than 95% for CO product. The work presents a temperature-universal formation of single-atom sites, which provides a novel platform for unraveling the active sites in Zn SACs for CO2 electroreduction and extends the synthesis of SACs with controllable coordination sites.

acidic CO2 electroreduction coordination evolution single-atom anchoring thermal-controlled atomization

SCI ; EI

英语

其他

Westlake Education Foundation[103506022001] ; Westlake University-Muyuan Joint Research Institute[206006022007] ; Zhejiang Provincial Natural Science Foundation of China[LQ20C030002] ; National Key Research and Development Project[2022YFA1503900] ; Shenzhen fundamental research funding["JCYJ20210324115809026","JCYJ20200109141216566","JCYJ20220818100212027"] ; Guangdong scientific program[2019QN01L057] ; null[2023M743372] ; null[GZC202325]

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

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

WOS:001248818000001

WILEY-V C H VERLAG GMBH

MATERIALS SCIENCE

Web of Science

1.Zhejiang Univ, Sch Mat Sci & Engn, Hangzhou 310027, Zhejiang, Peoples R China
2.Westlake Univ, Sch Engn, Hangzhou 310030, Zhejiang, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
4.Eastern Inst Technol, Eastern Inst Adv Study, Ningbo 315200, Zhejiang, Peoples R China
5.Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Jilin, Peoples R China
6.Univ Sci & Technol China, Sch Appl Chem & Engn, Hefei 230026, Anhui, Peoples R China
7.Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
8.Univ Sci & Technol China, iChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Synchrotron Radiat Lab, Key Lab Precis & Intelligent Chem, Hefei 230026, Anhui, Peoples R China
9.Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China
10.Jilin Univ, Key Lab Automobile Mat, Minist Educ, Changchun 130022, Jilin, Peoples R China
11.Jilin Univ, Coll Mat Sci & Engn, Changchun 130022, Jilin, Peoples R China
12.CALTECH, Dept Environm Sci & Engn, 1200 E Calif Blvd, Pasadena, CA 91125 USA
13.Beijing Normal Univ, Management Innovat Res Ctr, Zhuhai 519087, Guangdong, Peoples R China

Hao, Qi,Zhen, Cheng,Tang, Qi,et al. Universal Formation of Single Atoms from Molten Salt for Facilitating Selective CO₂ Reduction[J]. ADVANCED MATERIALS,2024.

Hao, Qi.,Zhen, Cheng.,Tang, Qi.,Wang, Jiazhi.,Ma, Peiyu.,...&Lu, Jun.(2024).Universal Formation of Single Atoms from Molten Salt for Facilitating Selective CO₂ Reduction.ADVANCED MATERIALS.

Hao, Qi,et al."Universal Formation of Single Atoms from Molten Salt for Facilitating Selective CO₂ Reduction".ADVANCED MATERIALS (2024).