Abstract
CO2 reduction reactions (CO2RR) powered by renewable electricity can directly convert CO2 to hydrocarbons and fix the intermittent sustainable energy in portable chemical fuels. It is of great importance to develop advanced catalysts that can boost CO2RR with high activity, selectivity, and efficiency at low overpotentials. Here, we report the solution synthesis using H2O2 to modify the surface structures of gold multi-twinned nanoparticles (AuMPs) and create tensile surface steps. Calculations predicted significantly enhanced CO2 adsorption and boosted CO2RR capabilities with inhibited hydrogen evolution reaction activity for the tensile surface steps with modified electronic structure. The H2O2-treated AuMPs with surface steps and 3.83% tensile lattices showed much higher activity and selectivity at lower overpotentials for CO2RR than pristine gold nanoparticles. The CO-production current density reached about 98 mA cm−2 with a Faradaic efficiency of 95.7% at −0.30 V versus reversible hydrogen electrode in the flow cell, showing a half-cell energy efficiency as high as ∼83%. Our strategy represents a rational catalyst design by engineering the surface structures of metal nanoparticles and may find more applicability in future electrocatalysis.
Article PDF
Similar content being viewed by others
Avoid common mistakes on your manuscript.
References
Gao D, Zhou H, Wang J, Miao S, Yang F, Wang G, Wang J, Bao X. J Am Chem Soc, 2015, 137: 4288–4291
Liu S, Tao H, Zeng L, Liu Q, Xu Z, Liu Q, Luo JL. J Am Chem Soc, 2017, 139: 2160–2163
Gu J, Hsu CS, Bai L, Chen HM, Hu X. Science, 2019, 364: 1091–1094
Asadi M, Kim K, Liu C, Addepalli AV, Abbasi P, Yasaei P, Phillips P, Behranginia A, Cerrato JM, Haasch R, Zapol P, Kumar B, Klie RF, Abiade J, Curtiss LA, Salehi-Khojin A. Science, 2016, 353: 467–470
Jiang K, Siahrostami S, Akey AJ, Li Y, Lu Z, Lattimer J, Hu Y, Stokes C, Gangishetty M, Chen G, Zhou Y, Hill W, Cai WB, Bell D, Chan K, Nørskov JK, Cui Y, Wang H. Chem, 2017, 3: 950–960
Ross MB, De Luna P, Li Y, Dinh CT, Kim D, Yang P, Sargent EH. Nat Catal, 2019, 2: 648–658
Goyal A, Marcandalli G, Mints VA, Koper MTM. J Am Chem Soc, 2020, 142: 4154–4161
Sun K, Cheng T, Wu L, Hu Y, Zhou J, Maclennan A, Jiang Z, Gao Y, Goddard Iii WA, Wang Z. J Am Chem Soc, 2017, 139: 15608–15611
Kim D, Resasco J, Yu Y, Asiri AM, Yang P. Nat Commun, 2014, 5: 4948
Fang Y, Flake JC. J Am Chem Soc, 2017, 139: 3399–3405
Trindell JA, Clausmeyer J, Crooks RM. J Am Chem Soc, 2017, 139: 16161–16167
Chen Y, Li CW, Kanan MW. J Am Chem Soc, 2012, 134: 19969–19972
Zhu W, Michalsky R, Metin Ö, Lv H, Guo S, Wright CJ, Sun X, Peterson AA, Sun S. J Am Chem Soc, 2013, 135: 16833–16836
Zhu W, Zhang YJ, Zhang H, Lv H, Li Q, Michalsky R, Peterson AA, Sun S. J Am Chem Soc, 2014, 136: 16132–16135
Feng X, Jiang K, Fan S, Kanan MW. J Am Chem Soc, 2015, 137: 4606–4609
Liu M, Pang Y, Zhang B, De Luna P, Voznyy O, Xu J, Zheng X, Dinh CT, Fan F, Cao C, de Arquer FPG, Safaei TS, Mepham A, Klinkova A, Kumacheva E, Filleter T, Sinton D, Kelley SO, Sargent EH. Nature, 2016, 537: 382–386
Liu Q, Yang X, Li L, Miao S, Li Y, Li Y, Wang X, Huang Y, Zhang T. Nat Commun, 2017, 8: 1407
Mariano RG, McKelvey K, White HS, Kanan MW. Science, 2017, 358: 1187–1192
Li J, Chen G, Zhu Y, Liang Z, Pei A, Wu CL, Wang H, Lee HR, Liu K, Chu S, Cui Y. Nat Catal, 2018, 1: 592–600
Liu M, Liu M, Wang X, Kozlov SM, Cao Z, De Luna P, Li H, Qiu X, Liu K, Hu J, Jia C, Wang P, Zhou H, He J, Zhong M, Lan X, Zhou Y, Wang Z, Li J, Seifitokaldani A, Dinh CT, Liang H, Zou C, Zhang D, Yang Y, Chan TS, Han Y, Cavallo L, Sham TK, Hwang BJ, Sargent EH. Joule, 2019, 3: 1703–1718
Yuan X, Zhang L, Li L, Dong H, Chen S, Zhu W, Hu C, Deng W, Zhao ZJ, Gong J. J Am Chem Soc, 2019, 141: 4791–4794
Cao Z, Kim D, Hong D, Yu Y, Xu J, Lin S, Wen X, Nichols EM, Jeong K, Reimer JA, Yang P, Chang CJ. J Am Chem Soc, 2016, 138: 8120–8125
Gao D, Zhang Y, Zhou Z, Cai F, Zhao X, Huang W, Li Y, Zhu J, Liu P, Yang F, Wang G, Bao X. J Am Chem Soc, 2017, 139: 5652–5655
Tang C, Shi J, Bai X, Hu A, Xuan N, Yue Y, Ye T, Liu B, Li P, Zhuang P, Shen J, Liu Y, Sun Z. ACS Catal, 2020, 10: 2026–2032
Cheng H, Yang N, Liu G, Ge Y, Huang J, Yun Q, Du Y, Sun CJ, Chen B, Liu J, Zhang H. Adv Mater, 2020, 32: 1902964
Li Z, Fu JY, Feng Y, Dong CK, Liu H, Du XW. Nat Catal, 2019, 2: 1107–1114
Wang H, Xu S, Tsai C, Li Y, Liu C, Zhao J, Liu Y, Yuan H, Abild-Pedersen F, Prinz FB, Nørskov JK, Cui Y. Science, 2016, 354: 1031–1036
Xia Y, Xiong Y, Lim B, Skrabalak SE. Angew Chem Int Ed, 2009, 48: 60–103
Ma Y, Zeng J, Li W, McKiernan M, Xie Z, Xia Y. Adv Mater, 2010, 22: 1930–1934
Walsh MJ, Yoshida K, Kuwabara A, Pay ML, Gai PL, Boyes ED. Nano Lett, 2012, 12: 2027–2031
Nørskov JK, Bligaard T, Rossmeisl J, Christensen CH. Nat Chem, 2009, 1: 37–46
Huang H, Jia H, Liu Z, Gao P, Zhao J, Luo Z, Yang J, Zeng J. Angew Chem Int Ed, 2017, 56: 3594–3598
Luo M, Zhao Z, Zhang Y, Sun Y, Xing Y, Lv F, Yang Y, Zhang X, Hwang S, Qin Y, Ma JY, Lin F, Su D, Lu G, Guo S. Nature, 2019, 574: 81–85
Ross MB, Dinh CT, Li Y, Kim D, De Luna P, Sargent EH, Yang P. J Am Chem Soc, 2017, 139: 9359–9363
Shi C, Hansen HA, Lausche AC, Nørskov JK. Phys Chem Chem Phys, 2014, 16: 4720–4727
Seh ZW, Kibsgaard J, Dickens CF, Chorkendorff I, Nørskov JK, Jaramillo TF. Science, 2017, 355: eaad4998
Yang HB, Hung SF, Liu S, Yuan K, Miao S, Zhang L, Huang X, Wang HY, Cai W, Chen R, Gao J, Yang X, Chen W, Huang Y, Chen HM, Li CM, Zhang T, Liu B. Nat Energy, 2018, 3: 140–147
Kresse G, Furthmüller J. Phys Rev B, 1996, 54: 11169–11186
Perdew JP, Burke K, Ernzerhof M. Phys Rev Lett, 1996, 77: 3865–3868
Hammer B, Hansen LB, Nørskov JK. Phys Rev B, 1999, 59: 7413–7421
Grimme S. J Comput Chem, 2006, 27: 1787–1799
Peterson AA, Abild-Pedersen F, Studt F, Rossmeisl J, Nørskov JK. Energy Environ Sci, 2010, 3: 1311–1315
Wang M, Shi H, Tian M, Chen R, Shu J, Zhang Q, Wang Y, Li C, Wan N, Lei S. ACS Appl Nano Mater, 2021, 4: 11017–11030
Wang M, Song R, Zhang Q, Li C, Xu Z, Liu G, Wan N, Lei S. Fuel, 2022, 321: 124101
Monzó J, Malewski Y, Kortlever R, Vidal-Iglesias FJ, Solla-Gullón J, Koper MTM, Rodriguez P. J Mater Chem A, 2015, 3: 23690–23698
Adit Maark T, Nanda BRK. J Phys Chem C, 2017, 121: 4496–4504
Jansonius RP, Reid LM, Virca CN, Berlinguette CP. ACS Energy Lett, 2019, 4: 980–986
Dinh CT, Burdyny T, Kibria MG, Seifitokaldani A, Gabardo CM, García de Arquer FP, Kiani A, Edwards JP, De Luna P, Bushuyev OS, Zou C, Quintero-Bermudez R, Pang Y, Sinton D, Sargent EH. Science, 2018, 360: 783–787
Luo M, Wang Z, Li YC, Li J, Li F, Lum Y, Nam DH, Chen B, Wicks J, Xu A, Zhuang T, Leow WR, Wang X, Dinh CT, Wang Y, Wang Y, Sinton D, Sargent EH. Nat Commun, 2019, 10: 5814
García de Arquer FP, Dinh CT, Ozden A, Wicks J, McCallum C, Kirmani AR, Nam DH, Gabardo C, Seifitokaldani A, Wang X, Li YC, Li F, Edwards J, Richter LJ, Thorpe SJ, Sinton D, Sargent EH. Science, 2020, 367: 661–666
Acknowledgements
We thank the Analytical and Testing Center of BIT for technical support. We acknowledge the financial support from the National Natural Science Foundation of China (21971012, 21922502, and 21971017), the National Key Research and Development Program of China (2020YFB1506300), the Beijing Municipal Natural Science Foundation (JQ20007), and the Beijing Institute of Technology Research Fund Program.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest The authors declare no conflict of interest.
Additional information
Supporting information The supporting information is available online at http://chem.scichina.com and http://springerlink.bibliotecabuap.elogim.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.
Rights and permissions
About this article
Cite this article
Chen, LW., Hao, YC., Li, J. et al. Multi-twinned gold nanoparticles with tensile surface steps for efficient electrocatalytic CO2 reduction. Sci. China Chem. 65, 2188–2196 (2022). https://doi.org/10.1007/s11426-022-1315-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11426-022-1315-x