Stabilization of Cu/Ni Alloy Nanoparticles with Graphdiyne Enabling Efficient CO₂ Reduction

Abstract

Electrocatalysis has become an attractive strategy for the artificial reduction of CO₂ to high-value chemicals. However, the design and development of highly selective and stable non-noble metal electrocatalysts that convert CO₂ to CO are still a challenge. As a new type of two-dimensional carbon material, graphdiyne(GDY), is rarely used to explore the application in carbon dioxide reduction reaction(CO₂RR). Therefore, we tried to use GDY as a substrate to stabilize the copper-nickel alloy nanoparticles(NPs) to synthesize Cu/Ni@GDY. Cu/Ni@GDY requires an overpotential (−0.61 V) to 10 mA/cm² for the formation of CO, and it shows better activity than Au and Ag, achieving a higher Faraday efficiency of about 95.2% and high stability of about 26 h at an overpotential (−0.70 V). The electronic interaction between GDY substrate and Cu/Ni alloy NPs and the large specific surface area of GDY is responsible for the high performance.

Keywords

Keywords Graphdiyne(GDY) / Carbon dioxide reduction reaction (CO₂RR) / CO / Electrocatalysis / Cu/Ni alloy nanoparticle

References

[1] Ringe S, Morales-Guio C G, Chen L D, Fields M, Jaramillo T F, Hahn C, Chan K. Nat. Commun., 2020, 11(1): 33.

[2] Bhargava S S, Proietto F, Azmoodeh D, Cofell E R, Henckel D A, Verma S, Brooks C J, Gewirth A A, Kenis P J A. Chem ElectroChem, 2020, 7(9): 2001.

[3] De Gregorio G L, Burdyny T, Loiudice A, Iyengar P, Smith W A, Buonsanti R. ACS Catal., 2020, 10(9): 4854.

[4] Li H, Liu T, Wei P, Lin L, Gao D, Wang G, Bao X. Angew Chem. Int. Ed. Engl., 2021, 60(26): 14329.

[5] Zhang B, Zhang J, Hua M, Wan Q, Su Z, Tan X, Liu L, Zhang F, Chen G, Tan D, Cheng X, Han B, Zheng L, Mo G. J. Am. Chem. Soc., 2020, 142(31): 13606.

[6] Li F, Thevenon A, Rosas-Hernandez A, Wang Z, Li Y, Gabardo C M, Ozden A, Dinh C T, Li J, Wang Y, Edwards J P, Xu Y, McCallum C, Tao L, Liang Z Q, Luo M, Wang X, Li H, O’Brien C P, Tan C S, Nam D H, Quintero-Bermudez R, Zhuang T T, Li Y C, Han Z, Britt R D, Sinton D, Agapie T, Peters J C, Sargent E H. Nature, 2020, 577(7791): 509.

[7] Huang J, Mensi M, Oveisi E, Mantella V, Buonsanti R. J. Am. Chem. Soc., 2019, 141(6): 2490.

[8] Rong W, Zou H, Zang W, Xi S, Wei S, Long B, Hu J, Ji Y, Duan L. Angew. Chem. Int. Ed. Engl., 2021, 60(1): 466.

[9] Wang Z L, Sun K, Henzie J, Hao X, Li C, Takei T, Kang Y M, Yamauchi Y. Angew. Chem. Int. Ed. Engl., 2018, 57(20): 5848.

[10] Wang C, Guan E, Wang L, Chu X, Wu Z, Zhang J, Yang Z, Jiang Y, Zhang L, Meng X, Gates B C, Xiao F S. J. Am. Chem. Soc., 2019, 141(21): 8482.

[11] Li X, Yu J, Jia J, Wang A, Zhao L, Xiong T, Liu H, Zhou W. Nano Energy, 2019, 62: 127.

[12] Liu M, Liu M, Wang X, Kozlov S M, 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 C T, Liang H, Zou C, Zhang D, Yang Y, Chan T-S, Han Y, Cavallo L, Sham T-K, Hwang B-J, Sargent E H. Joule, 2019, 3(7): 1703.

[13] Wang F, Zuo Z, Shang H, Zhao Y, Li Y. ACS Appl. Mater. Interfaces, 2019, 11(3): 2599.

[14] Li J, Gao X, Zhu L, Ghazzal M N, Zhang J, Tung C-H, Wu L-Z. Energy Environ. Sci., 2020, 13(5): 1326.

[15] Hui L, Xue Y, Yu H, Liu Y, Fang Y, Xing C, Huang B, Li Y. J. Am. Chem. Soc., 2019, 141(27): 10677.

[16] Li J, Gao X, Liu B, Feng Q, Li X B, Huang M Y, Liu Z, Zhang J, Tung C H, Wu L Z. J. Am. Chem. Soc., 201, 138(12): 3954.

[17] Qi H, Yu P, Wang Y, Han G, Liu H, Yi Y, Li Y, Mao L. J. Am. Chem. Soc., 2015, 137(16): 5260.

[18] Fang Y, Xue Y, Hui L, Yu H, Liu Y, Xing C, Lu F, He F, Liu H, Li Y. Nano Energy, 2019, 59: 591.

[19] Ma X, Qi K, Wei S, Zhang L, Cui X. J. Alloys Compd., 2019, 770: 236.

[20] Zhang S, Liu H, Huang C, Cui G, Li Y. Chem. Commun. (Camb), 2015, 51(10): 1834.

[21] Shi G, Xie Y, Du L, Fan Z, Chen X, Fu X, Xie W, Wang M, Yuan M. Nano Energy, 2020, 74: 104852.

[22] Shi G, Fan Z, Du L, Fu X, Dong C, Xie W, Zhao D, Wang M, Yuan M. Mater. Chem. Front., 2019, 3(5): 821.

[23] Zhu D D, Liu J L, Qiao S Z. Adv. Mater., 201, 28(18): 3423.