Engineering of Coordination Environment and Multiscale Structure in Single-Site Copper Catalyst for Superior Electrocatalytic Oxygen Reduction

Sun，Tingting1,2; Li，Yinlong3; Cui，Tingting2; Xu，Lianbin4; Wang，Yang Gang3; Chen，Wenxing5; Zhang，Pianpian1; Zheng，Tianyu1; Fu，Xianzhang1; Zhang，Shaolong2; Zhang，Zedong2; Wang，Dingsheng2; Li，Yadong2

2020-08-12

10.1021/acs.nanolett.0c02677

NANO LETTERS   影响因子和分区

1530-6984

1530-6992

Herein, we report efficient single copper atom catalysts that consist of dense atomic Cu sites dispersed on a three-dimensional carbon matrix with highly enhanced mesoporous structures and improved active site accessibility (Cu-SA/NC(meso)). The ratio of +1 to +2 oxidation state of the Cu sites in the Cu-SA/NC(meso) catalysts can be controlled by varying the urea content in the adsorption precursor, and the activity for ORR increases with the addition of Cu1+ sites. The optimal Cu1+-SA/NC(meso)-7 catalyst with highly accessible Cu1+ sites exhibits superior ORR activity in alkaline media with a half-wave potential (E1/2) of 0.898 V vs RHE, significantly exceeding the commercial Pt/C, along with high durability and enhanced methanol tolerance. Control experiments and theoretical calculations demonstrate that the superior ORR catalytic performance of Cu1+-SA/NC(meso)-7 catalyst is attributed to the atomically dispersed Cu1+ sites in catalyzing the reaction and the advantage of the introduced mesoporous structure in enhancing the mass transport.

copper mesoporous structure oxidation state oxygen reduction reaction Single atoms

SCI ; EI

英语

NI论文 ; ESI高被引

其他

National Key R&D Program of China[2018YFA0702003][2016YFA0202801] ; National Natural Science Foundation of China[21890383][21671117][21871159][21676018] ; Science and Technology Key Project of Guangdong Province of China[2020B010188002] ; Beijing Municipal Science & Technology Commission[Z191100007219003] ; Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology (SUSTech), China[2020B121201002]

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

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

WOS:000562935200086

AMER CHEMICAL SOC

20203709166746

Mesoporous materials ; Oxygen ; Coordination reactions ; Electrolytic reduction ; Urea ; Atoms ; Catalyst activity

Ore Treatment:533.1 ; Copper:544.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Atomic and Molecular Physics:931.3

MATERIALS SCIENCE

2-s2.0-85089615318

Scopus

1.Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials,Department of Chemistry,University of Science and Technology Beijing,100083,China
2.Department of Chemistry,Tsinghua University,100084,China
3.Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
4.State Key Laboratory of Organic-Inorganic Composites,Beijing University of Chemical Technology,100029,China
5.Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications,School of Materials Science and Engineering,Beijing Institute of Technology,100081,China

Sun，Tingting,Li，Yinlong,Cui，Tingting,et al. Engineering of Coordination Environment and Multiscale Structure in Single-Site Copper Catalyst for Superior Electrocatalytic Oxygen Reduction[J]. NANO LETTERS,2020,20(8):6206-6214.

Sun，Tingting.,Li，Yinlong.,Cui，Tingting.,Xu，Lianbin.,Wang，Yang Gang.,...&Li，Yadong.(2020).Engineering of Coordination Environment and Multiscale Structure in Single-Site Copper Catalyst for Superior Electrocatalytic Oxygen Reduction.NANO LETTERS,20(8),6206-6214.

Sun，Tingting,et al."Engineering of Coordination Environment and Multiscale Structure in Single-Site Copper Catalyst for Superior Electrocatalytic Oxygen Reduction".NANO LETTERS 20.8(2020):6206-6214.