化工进展 ›› 2024, Vol. 43 ›› Issue (6): 3174-3186.DOI: 10.16085/j.issn.1000-6613.2023-0857
• 材料科学与技术 • 上一篇
收稿日期:
2023-05-25
修回日期:
2023-07-11
出版日期:
2024-06-15
发布日期:
2024-07-02
通讯作者:
刘祥春,崔平
作者简介:
蔚德磊(1987—),男,博士研究生,研究方向为CO2电化学还原。E-mail:yudelei@ahut.edu.cn。
基金资助:
YU Delei(), HAN Kangshun, CHEN Yao, LIU Xiangchun(
), CUI Ping(
)
Received:
2023-05-25
Revised:
2023-07-11
Online:
2024-06-15
Published:
2024-07-02
Contact:
LIU Xiangchun, CUI Ping
摘要:
单原子Ni、N共掺杂碳材料基催化剂(Ni-N-C)电催化CO2制CO,因其在较大的电流密度和较大的过电势下仍具有超高的CO选择性,引起了广泛关注。本文综述了Ni-N-C电催化CO2制CO研究进展,包括氮掺杂碳材料基催化剂和Ni-N-C电催化CO2制CO。总结了氮掺杂碳材料基催化剂中不同形态N的催化活性,目前为止,N在该类催化剂电化学还原CO2中的确切作用没有达成共识。此外,还总结了Ni-N-C的催化性能、催化机理及催化性能改性方法,探讨了与Ni配位的N原子和缺陷位对催化活性的影响规律,分析了各类碳载体的优缺点。Ni-N-C电化学还原CO2制CO研究已取得一定的进展,如电流密度可达工业级要求,但是其实现大规模工业化应用还需解决一些关键问题,如开发高活性和高稳定性Ni-N-C的定向制备技术;研发制备简易温和、成本低廉、具有抗腐蚀性、耐高温的先进碳载体材料。
中图分类号:
蔚德磊, 韩康顺, 陈瑶, 刘祥春, 崔平. 单原子Ni、N共掺杂碳材料基催化剂电还原CO2制CO研究进展[J]. 化工进展, 2024, 43(6): 3174-3186.
YU Delei, HAN Kangshun, CHEN Yao, LIU Xiangchun, CUI Ping. Recent advances in electroreduction of CO2 to CO using single atom Ni, N co-doped carbon-material based catalysts[J]. Chemical Industry and Engineering Progress, 2024, 43(6): 3174-3186.
图10 CO2还原活性位点的结构演变[105](ΔD表示Ni原子向CO2电子转移产生的Ni原子离开平面的位移;右上角的示意图显示了Ni(Ⅰ)活性位点上CO2分子的活化过程;红色箭头表示从Ni(Ⅰ)到吸附的CO2的电子转移。EF1和EF2分别是形成Ni-CO2δ- 之前和之后的Ni-N-C的费米能级;1πg和2πu是CO2的分子轨道)
制备方法 | 碳材料载体或其前体 | 电化学性能 | 参考文献 | |
---|---|---|---|---|
电解液 | 性能参数 | |||
900℃煅烧 | 改性石墨烯 | 0.1mol/L KHCO3 | FECO=90% @ -0.7~-0.9V(vs.RHE);TOF=2700h-1 @ -0.7V(vs.RHE); 稳定运行时长> 5h @ -0.65V(vs.RHE);塔菲尔斜率=126mV/dec | [ |
750℃煅烧 | 石墨烯纳米片 | 0.5mol/L KHCO3 | FECO=95%、电流密度=11mA/cm2 @ 620 mV;TOF = 6.8s-1 @ 0.57V; 稳定运行时长> 20h @ 12mA/cm2;塔菲尔斜率=110mV/dec | [ |
分子工程法引入甲氧基、1000℃煅烧 | 碳纳米管 | 1mol/L KHCO3 | FECO=99.5% @ 电流密度=10~300mA/cm2; TOF = 2.9s-1 @ -0.64V(vs.RHE);稳定运行时长> 40h @ 150mA/cm2 | [ |
微波诱导等离子体法引入S原子 | 氧化石墨烯 | 0.5mol/L KHCO3 | FECO=97%、电流密度=40mA/cm2@ -0.8~-0.9V(vs.RHE); TOF = 3965h-1 @ -0.79V(vs.RHE);稳定运行时长> 20h @ -0.8V | [ |
氰基修饰碳基底、670℃煅烧 | C3N4 | 0.5mol/L KHCO3 | FECO≥90% @ -0.58~-1.18V(vs.RHE);电流密度=46.8mA/cm2、 TOF = 22000h-1 @ -1.18V;稳定运行时长> 12h @ -0.88V(vs.RHE) | [ |
800~1000℃煅烧、模板法 | 多巴胺 | 0.5mol/L KHCO3 | FECO=96%、电流密度=35mA/cm2@ -1V(vs.RHE); 稳定运行时长>12h @ 2.4V | [ |
400~1000℃煅烧 | ZIF-8 | 0.5mol/L KHCO3 | FECO=92%、电流密度=92.1mA/cm2、TOF = 5500h-1 @ -0.9V(vs.RHE); 稳定运行时长> 70h @ -0.6V(vs.RHE) | [ |
1000℃煅烧 | ZIF-8 | 0.5mol/L KHCO3 | FECO=71.9%、电流密=10.48mA/cm2、TOF = 5273h-1 @ -0.89V; 稳定运行时长>60h @ -1.0V(vs.RHE);塔菲尔斜率=249mV/dec | [ |
静电纺丝法、750℃煅烧 | 石墨壳 | 0.1mol/L KHCO3 | FECO=93.2%、电流密度=4mA/cm2、稳定运行时长>20h @ -0.7V; 塔菲尔斜率=138.5mV/dec | [ |
拓扑化学转化法 | 葡萄糖、C3N4 | 0.5mol/L KHCO3 | FECO>90% @ -0.5~-0.9V;电流密度=28.6mA/cm2@ -0.81V; 塔菲尔斜率=103mV/dec | [ |
850℃煅烧 | 碳纳米管 | 0.5mol/L KHCO3 | FECO=97% @ -0.83V(vs.RHE);TOF =13860h-1、电流密度=17.5mA/cm2@ -0.94 V(vs.RHE);稳定运行时长>16h @ -0.79V(vs.RHE) | [ |
后离子交换法、900℃煅烧 | ZIF-8 | 0.5mol/L KHCO3 | FECO=95.6%、TOF=1425 h-1、电流密度=6.64mA/cm2、 稳定运行时长>10h @ -0.65V;塔菲尔斜率=99mV/dec | [ |
950℃煅烧 | 三(4-氨苯基)胺为原料制备酶 | 0.5mol/L KHCO3 | FECO=99.6%、电流密度=1.23A/cm2、TOF =69.7s-1 @ -2.4V(vs.RHE); 稳定运行时长>100h @ -2.2 V(vs.RHE) | [ |
静电纺丝法、1000℃煅烧 | 聚丙烯腈、聚苯乙烯 | 0.5mol/L KHCO3 | FECO=96.6% @ -0.8 V(vs.RHE);电流密度=15.5mA/cm2、 TOF=4606.5h-1 @ -1.0V;塔菲尔斜率=124.6mV/dec | [ |
600~800℃煅烧 | 苯代三聚氰胺、 氰尿酸 | 0.5mol/L KHCO3 | FECO>90%、电流密度=65mA/cm2、TOF=135000h-1 @ -0.9V(vs.RHE); 稳定运行时长>14h @ -0.7V(vs.RHE);塔菲尔斜率=124mV/dec | [ |
900℃煅烧、引入S原子 | 石墨烯 | 0.5mol/L KHCO3 | FECO=97%、电流密度=350A/gcatalyst、TOF = 14800h-1、 稳定运行时长>100h @ 0.61V;塔菲尔斜率=114mV/dec | [ |
600℃、1000℃煅烧 | 炭黑 | 0.5mol/L KHCO3 | FECO >95% @ -0.6~-0.84V(vs.RHE);电流密度=21mA/cm2 @ -0. 9V (vs.RHE);稳定运行时长>24h @ 0.55V;塔菲尔斜率=101mV/dec | [ |
静电纺丝法、900℃煅烧 | 多孔碳纤维薄膜 | 0.5mol/L KHCO3 | FECO=96%、电流密度=56.1mA/cm2 @ -0.7V(vs.RHE); 塔菲尔斜率=117mV/dec | [ |
表1 典型Ni-N-C的制备方法及其在H型电解池中催化性能总结
制备方法 | 碳材料载体或其前体 | 电化学性能 | 参考文献 | |
---|---|---|---|---|
电解液 | 性能参数 | |||
900℃煅烧 | 改性石墨烯 | 0.1mol/L KHCO3 | FECO=90% @ -0.7~-0.9V(vs.RHE);TOF=2700h-1 @ -0.7V(vs.RHE); 稳定运行时长> 5h @ -0.65V(vs.RHE);塔菲尔斜率=126mV/dec | [ |
750℃煅烧 | 石墨烯纳米片 | 0.5mol/L KHCO3 | FECO=95%、电流密度=11mA/cm2 @ 620 mV;TOF = 6.8s-1 @ 0.57V; 稳定运行时长> 20h @ 12mA/cm2;塔菲尔斜率=110mV/dec | [ |
分子工程法引入甲氧基、1000℃煅烧 | 碳纳米管 | 1mol/L KHCO3 | FECO=99.5% @ 电流密度=10~300mA/cm2; TOF = 2.9s-1 @ -0.64V(vs.RHE);稳定运行时长> 40h @ 150mA/cm2 | [ |
微波诱导等离子体法引入S原子 | 氧化石墨烯 | 0.5mol/L KHCO3 | FECO=97%、电流密度=40mA/cm2@ -0.8~-0.9V(vs.RHE); TOF = 3965h-1 @ -0.79V(vs.RHE);稳定运行时长> 20h @ -0.8V | [ |
氰基修饰碳基底、670℃煅烧 | C3N4 | 0.5mol/L KHCO3 | FECO≥90% @ -0.58~-1.18V(vs.RHE);电流密度=46.8mA/cm2、 TOF = 22000h-1 @ -1.18V;稳定运行时长> 12h @ -0.88V(vs.RHE) | [ |
800~1000℃煅烧、模板法 | 多巴胺 | 0.5mol/L KHCO3 | FECO=96%、电流密度=35mA/cm2@ -1V(vs.RHE); 稳定运行时长>12h @ 2.4V | [ |
400~1000℃煅烧 | ZIF-8 | 0.5mol/L KHCO3 | FECO=92%、电流密度=92.1mA/cm2、TOF = 5500h-1 @ -0.9V(vs.RHE); 稳定运行时长> 70h @ -0.6V(vs.RHE) | [ |
1000℃煅烧 | ZIF-8 | 0.5mol/L KHCO3 | FECO=71.9%、电流密=10.48mA/cm2、TOF = 5273h-1 @ -0.89V; 稳定运行时长>60h @ -1.0V(vs.RHE);塔菲尔斜率=249mV/dec | [ |
静电纺丝法、750℃煅烧 | 石墨壳 | 0.1mol/L KHCO3 | FECO=93.2%、电流密度=4mA/cm2、稳定运行时长>20h @ -0.7V; 塔菲尔斜率=138.5mV/dec | [ |
拓扑化学转化法 | 葡萄糖、C3N4 | 0.5mol/L KHCO3 | FECO>90% @ -0.5~-0.9V;电流密度=28.6mA/cm2@ -0.81V; 塔菲尔斜率=103mV/dec | [ |
850℃煅烧 | 碳纳米管 | 0.5mol/L KHCO3 | FECO=97% @ -0.83V(vs.RHE);TOF =13860h-1、电流密度=17.5mA/cm2@ -0.94 V(vs.RHE);稳定运行时长>16h @ -0.79V(vs.RHE) | [ |
后离子交换法、900℃煅烧 | ZIF-8 | 0.5mol/L KHCO3 | FECO=95.6%、TOF=1425 h-1、电流密度=6.64mA/cm2、 稳定运行时长>10h @ -0.65V;塔菲尔斜率=99mV/dec | [ |
950℃煅烧 | 三(4-氨苯基)胺为原料制备酶 | 0.5mol/L KHCO3 | FECO=99.6%、电流密度=1.23A/cm2、TOF =69.7s-1 @ -2.4V(vs.RHE); 稳定运行时长>100h @ -2.2 V(vs.RHE) | [ |
静电纺丝法、1000℃煅烧 | 聚丙烯腈、聚苯乙烯 | 0.5mol/L KHCO3 | FECO=96.6% @ -0.8 V(vs.RHE);电流密度=15.5mA/cm2、 TOF=4606.5h-1 @ -1.0V;塔菲尔斜率=124.6mV/dec | [ |
600~800℃煅烧 | 苯代三聚氰胺、 氰尿酸 | 0.5mol/L KHCO3 | FECO>90%、电流密度=65mA/cm2、TOF=135000h-1 @ -0.9V(vs.RHE); 稳定运行时长>14h @ -0.7V(vs.RHE);塔菲尔斜率=124mV/dec | [ |
900℃煅烧、引入S原子 | 石墨烯 | 0.5mol/L KHCO3 | FECO=97%、电流密度=350A/gcatalyst、TOF = 14800h-1、 稳定运行时长>100h @ 0.61V;塔菲尔斜率=114mV/dec | [ |
600℃、1000℃煅烧 | 炭黑 | 0.5mol/L KHCO3 | FECO >95% @ -0.6~-0.84V(vs.RHE);电流密度=21mA/cm2 @ -0. 9V (vs.RHE);稳定运行时长>24h @ 0.55V;塔菲尔斜率=101mV/dec | [ |
静电纺丝法、900℃煅烧 | 多孔碳纤维薄膜 | 0.5mol/L KHCO3 | FECO=96%、电流密度=56.1mA/cm2 @ -0.7V(vs.RHE); 塔菲尔斜率=117mV/dec | [ |
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