@article{cab67efd8fc642aeb6fe1b1272f616d2,
title = "Quantum-Dot-Derived Catalysts for CO2 Reduction Reaction",
abstract = "Defect sites are often proposed as key active sites in the design of catalysts. A promising strategy for improving activity is to achieve a high density of homogeneously dispersed atomic defects; however, this is seldom accomplished in metals. We hypothesize that vacancy-rich catalysts could be obtained through the synthesis of quantum dots (QDs) and their electrochemical reduction during the CO2 reduction reaction (CO2RR). Here, we report that QD-derived catalysts (QDDCs) with up to 20 vol % vacancies achieve record current densities of 16, 19, and 25 mAcm−2 with high faradic efficiencies in the electrosynthesis of formate, carbon monoxide, and ethylene at low potentials of –0.2, –0.3, and –0.9 V versus reversible hydrogen electrode (RHE), respectively. The materials are stable after 80 hr of CO2RR. These CO2RR performances in aqueous solution surpass those of previously reported catalysts by 2×. Together, X-ray absorption spectroscopy and computational studies reveal that the vacancies produce a local atomic and electronic structure that enhances CO2RR.",
author = "Min Liu and Mengxia Liu and Xiaoming Wang and Sergey Kozlov and Zhen Cao and {De Luna}, Phil and Hongmei Li and Xiaoqing Qiu and Kang Liu and Junhua Hu and Chuankun Jia and Peng Wang and Huimin Zhou and Jun He and Miao Zhong and Xinzheng Lan and Yansong Zhou and Zhiqiang Wang and Jun Li and Ali Seifitokaldani and Dinh, {Cao Thang} and Hongyan Liang and Chengqin Zou and Daliang Zhang and Yang Yang and Chan, {Ting Shan} and Yu Han and Luigi Cavallo and Sham, {Tsun Kong} and Hwang, {Bing Joe} and Sargent, {Edward H.}",
note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This work was supported financially by the National Natural Science Foundation of China (21872174), International S&T Cooperation Program of China (2017YFE0127800), the Ontario Research Fund Research-Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, the Canadian Institute for Advanced Research Bio-inspired Solar Energy program, a University of Toronto Connaught grant, the Ministry of Science and Technology of Taiwan, the King Abdullah University of Science and Technology (KAUST), the Project of Innovation-Driven Plan in Central South University (2017CX003, 20180018050001), the Hunan Provincial Science and Technology Program (2017XK2026), the State Key Laboratory of Powder Metallurgy in Central South University, the Shenzhen Science and Technology Innovation Project (JCYJ20180307151313532, JCYJ20180307164633296), the Thousand Youth Talents Plan of China, and the Hundred Youth Talents Program of Hunan. S.M.K. Z.C. and L.C. thank the KAUST Supercomputing Laboratory for the resources provided. This work benefited from Taiwan Beam Lines BL01C1, BL07A1, and BL17C1 in the National Synchrotron Radiation Research Center, the Soft X-Ray Microcharacterization Beamline at Canadian Light Source (CLS) and Sector 20-BM at the Advanced Photon Source (APS). The authors thank Y. Pang, J. Fan, O.Voznyy, J. Xu, F. Arquer, T. Safaei, A. Klinkova, R. Wolowiec, D. Kopilovic, L. Levina, J. Tam, S. Boccia, and S. Hoogland from U of T for fruitful discussions; Y. Hu from CLS; Z. Finfrock and M. Ward from APS; and C. Xiao from the University of Science and Technology of China for their help during the study. Min Liu, E.H.S. and B.-J.H. supervised the project. Min Liu, Mengxia Liu, and X.W. designed the experiments. S.M.K. Z.C. and L.C. carried out electrochemical simulations. S.M.K. Z.C. and L.C. carried out electrochemical simulations. P.D.L. and A.S. carried out simulations of vacancy formation energies. Mengxia Liu, X.L. P.W. and H.L. synthesized quantum dots and did ligand exchange. Min Liu, X.W. Z.W. T.-S.C. T.-K.S. and B.-J.H. performed the X-ray measurements. Y.Y. carried out in situ Raman measurements. D.Z. and Y.H. performed the TEM measurements. H.L. and K.L. carried out the XPS measurements. X.Q. J.H, C.J. H.Z. M.Z. Y.Z. C.T.D. and C.Z. performed electrochemical measurements. All authors discussed the results and assisted during manuscript preparation. The authors declare no competing interests.",
year = "2019",
month = jun,
day = "25",
doi = "10.1016/j.joule.2019.05.010",
language = "English (US)",
volume = "3",
pages = "1703--1718",
journal = "Joule",
issn = "2542-4351",
publisher = "Cell Press",
number = "7",
}