Carbonized Yolk-shell Metal-Organic Frameworks for Electrochemical Conversion of CO₂ into Ethylene

Abstract

With the excessive consumption of fossil fuels and the massive emission of CO₂, it has led to a series of environmental crises posing a serious threat to sustainable development. Electrochemical CO₂ reduction reaction (CO₂RR) to ethylene helps solve these serious environmental crises. Herein, we report the synthesis of a copper-based electrocatalyst by pyrolysis of yolk-shell structured HKUST-1 with partial substitution of trimesic acid by benzimidazole(nitrogen source). The electrocatalyst exhibits an ethylene Faradic efficiency(FE) of 25.8% and a partial ethylene current density of 23.7 mA/cm², in addition, the electrocatalyst can maintain stable performance during 10 h of electrolysis, which are all better than those of the electrocatalyst without nitrogen dopant. According to electrochemical measurements and X-ray photoelectron spectroscopy(XPS), we propose that the nitrogen dopant plays an effective role in stabilizing Cu(I) species and promoting CO₂ molecules activation, as well as suppressing the reduction of Cu(I) species during electrolysis. Eventually, the performance of the electrocatalyst toward CO₂RR is studied in a flow cell. This work provides a new route for the design of Cu-based electrocatalyst toward electrochemical CO₂ conversion into ethylene.

Keywords

CO₂ / Cu MOF / Electrocatalyst / Nitrogen / Ethylene

References

[1] Tan X, Yu C, Ren Y, Cui S, Li W, Qiu J. Energy Environ. Sci., 2021, 14(2): 765.

[2] Quan Y, Zhu J, Zheng G. Small Sci., 2021, 1(10): 2100043.

[3] Song R-B, Zhu W, Fu J, Chen Y, Liu L, Zhang J-R, Lin Y, Zhu J-J. Adv. Mater., 2020, 32(27): 1903796.

[4] Liu R, Shuai X S, Hao G-P, Lu A-H. Chem. Res. Chinese Universities, 2022, 38(1): 18.

[5] Xiao D J, Chant E D, Frankhouser A D, Chen Y, Yau A, Washton N M, Kanan M W. Nat. Chem., 2019, 11(10): 940.

[6] Sun L, Reddu V, Fisher A C, Wang X. Energy Environ. Sci., 2020, 13(2): 374.

[7] Wang G, Chen J, Ding Y, Cai P, Yi L, Li Y, Tu C, Hou Y, Wen Z, Dai L. Chem. Soc. Rev., 2021, 50(8): 4993.

[8] Seh Zhi W, Kibsgaard J, Dickens Colin F, Chorkendorff I, Nørskov Jens K, Jaramillo Thomas F. Science, 2017, 355(6321): eaad4998.

[9] Fan L, Xia C, Yang F, Wang J, Wang H, Lu Y. Sci. Adv., 2020, 6(8): eaay3111.

[10] Zhu W, Kattel S, Jiao F, Chen J G. Adv. Eng. Mater., 2019, 9(9): 1802840.

[11] Yang C, Chai J, Wang Z, Xing Y, Peng J, Yan Q. Chem. Res. Chinese Universities, 2020, 36(3): 410.

[12] Abeyweera S C, Yu J, Perdew J P, Yan Q, Sun Y. Nano Lett., 2020, 20(4): 2806.

[13] Zheng T, Jiang K, Ta N, Hu Y, Zeng J, Liu J, Wang H. Joule, 2019, 3(1): 265.

[14] Zhang X, Liu H, Qin J, Han H, Qiu C, Zhang S, Hao X, Liu W, Song Y. Chem. Commun., 2019, 55(39): 5659.

[15] Dinh C-T, Burdyny T, Kibria Md G, Seifitokaldani A, Gabardo Christine M, García de Arquer F P, Kiani A, Edwards Jonathan P, De Luna P, Bushuyev Oleksandr S, Zou C, Quintero-Bermudez R, Pang Y, Sinton D, Sargent Edward H. Science, 2018, 360(6390): 783.

[16] Fu X, Zhu A, Chen X, Zhang S, Wang M, Yuan M. Chem. Res. Chinese Universities, 2021, 37(6): 1328.

[17] Popović S, Smiljanić M, Jovanovič P, Vavra J, Buonsanti R, Hodnik N. Angew. Chem. Int. Ed., 2020, 59(35): 14736.

[18] Nitopi S, Bertheussen E, Scott S B, Liu X, Engstfeld A K, Horch S, Seger B, Stephens I E L, Chan K, Hahn C, Nørskov J K, Jaramillo T F, Chorkendorff I. Chem. Rev., 2019, 119(12): 7610.

[19] Shah S S A, Najam T, Wen M, Zang S-Q, Waseem A, Jiang H-L. Small Struct., 2021, 3(5): 2100090.

[20] Wu Y, Cao S, Hou J, Li Z, Zhang B, Zhai P, Zhang Y, Sun L. Adv. Eng. Mater., 2020, 10(29): 2000588.

[21] Wang S, Kou T, Baker S E, Duoss E B, Li Y. Mater. Today Nano, 2020, 12: 100096.

[22] Xiao H, Goddard William A, Cheng T, Liu Y. Proc. Natl. Acad. Sci., 2017, 114(26): 6685.

[23] Chou T-C, Chang C-C, Yu H-L, Yu W-Y, Dong C-L, Velasco-Vález J-J, Chuang C-H, Chen L-C, Lee J-F, Chen J-M, Wu H-L. J. Am. Chem. Soc., 2020, 142(6): 2857.

[24] Arán-Ais R M, Scholten F, Kunze S, Rizo R, Roldan Cuenya B. Nat. Energy, 2020, 5(4): 317.

[25] Kim J Y, Kim G, Won H, Gereige I, Jung W-B, Jung H-T. Adv. Mater., 2022, 34(3): 2106028.

[26] Zhou Y, Che F, Liu M, Zou C, Liang Z, De Luna P, Yuan H, Li J, Wang Z, Xie H, Li H, Chen P, Bladt E, Quintero-Bermudez R, Sham T-K, Bals S, Hofkens J, Sinton D, Chen G, Sargent E H. Nat. Chem., 2018, 10(9): 974.

[27] Wang X, Wang Z, García de Arquer F P, Dinh C-T, Ozden A, Li Y C, Nam D-H, Li J, Liu Y-S, Wicks J, Chen Z, Chi M, Chen B, Wang Y, Tam J, Howe J Y, Proppe A, Todorović P, Li F, Zhuang T-T, Gabardo C M, Kirmani A R, McCallum C, Hung S-F, Lum Y, Luo M, Min Y, Xu A, O’Brien C P, Stephen B, Sun B, Ip A H, Richter L J, Kelley S O, Sinton D, Sargent E H. Nat. Energy, 2020, 5(6): 478.

[28] Morales-Guio C G, Cave E R, Nitopi S A, Feaster J T, Wang L, Kuhl K P, Jackson A, Johnson N C, Abram D N, Hatsukade T, Hahn C, Jaramillo T F. Nat. Catal., 2018, 1(10): 764.

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

[30] Zhang W, Huang C, Xiao Q, Yu L, Shuai L, An P, Zhang J, Qiu M, Ren Z, Yu Y. J. Am. Chem. Soc., 2020, 142(26): 11417.

[31] Vasileff A, Zhu Y, Zhi X, Zhao Y, Ge L, Chen H M, Zheng Y, Qiao S-Z. Angew. Chem. Int. Ed., 2020, 59(44): 19649.

[32] Zhuang T-T, Pang Y, Liang Z-Q, Wang Z, Li Y, Tan C-S, Li J, Dinh C T, De Luna P, Hsieh P-L, Burdyny T, Li H-H, Liu M, Wang Y, Li F, Proppe A, Johnston A, Nam D-H, Wu Z-Y, Zheng Y-R, Ip A H, Tan H, Chen L-J, Yu S-H, Kelley S O, Sinton D, Sargent E H. Nat. Catal., 2018, 1(12): 946.

[33] Zhuang T-T, Liang Z-Q, Seifitokaldani A, Li Y, De Luna P, Burdyny T, Che F, Meng F, Min Y, Quintero-Bermudez R, Dinh C T, Pang Y, Zhong M, Zhang B, Li J, Chen P-N, Zheng X-L, Liang H, Ge W-N, Ye B-J, Sinton D, Yu S-H, Sargent E H. Nat. Catal., 2018, 1(6): 421.

[34] Karapinar D, Creissen C E, Rivera de la Cruz J G, Schreiber M W, Fontecave M. ACS Energy Letters, 2021, 6(2): 694.

[35] Liang Z-Q, Zhuang T-T, Seifitokaldani A, Li J, Huang C-W, Tan C-S, Li Y, De Luna P, Dinh C T, Hu Y, Xiao Q, Hsieh P-L, Wang Y, Li F, Quintero-Bermudez R, Zhou Y, Chen P, Pang Y, Lo S-C, Chen L-J, Tan H, Xu Z, Zhao S, Sinton D, Sargent E H. Nat. Commun., 2018, 9(1): 3828.

[36] Han X, He X, Sun L, Han X, Zhan W, Xu J, Wang X, Chen J. ACS Catal., 2018, 8(4): 3348.

[37] Lv Y, Liu H, Li J, Chen J, Song Y. J. Electroanal. Chem., 2020, 870: 114172.

[38] Lv Y, Liu H, Qin J, Gao R, Zhang Y, Xie Y, Li J, Song Y. Prog. Nat. Sci. Mater. Int., 2020, 30(6): 832.

[39] Han H, Y. W, Zhang Y, Cong Y, Qin J, Gao R, Chai C, Song Y. Acta Phys.-Chim. Sin., 2021, 37(9): 2008017.

[40] Chen L., Li Y., Xu N., Zhang G., Carbon, 2018, 132, 172

[41] Han X, He X, Wang F, Chen J, Xu J, Wang X, Han X. J. Mater. Chem. A, 2017, 5(21): 10220.

[42] Li Z, Yang Y, Yin Z, Wei X, Peng H, Lyu K, Wei F, Xiao L, Wang G, Abruña H D, Lu J, Zhuang L. ACS Catal., 2021, 11(5): 2473.

[43] Yuan J, Yang M-P, Zhi W-Y, Wang H, Wang H, Lu J-X. J. CO2 Util., 2019, 33: 452.

[44] Liu P, Hensen E J M. J. Am. Chem. Soc., 2013, 135(38): 14032.

[45] Platzman I, Brener R, Haick H, Tannenbaum R. J. Phys. Chem. C, 2008, 112(4): 1101.

[46] Lin S-C, Chang C-C, Chiu S-Y, Pai H-T, Liao T-Y, Hsu C-S, Chiang W-H, Tsai M-K, Chen H M. Nat. Commun., 2020, 11(1): 3525.

[47] Lee S, Kim D, Lee J. Angew. Chem. Int. Ed., 2015, 54(49): 14701.

[48] Bai X, Li Q, Shi L, Niu X, Ling C, Wang J. Small, 2020, 16(12): 1901981.