化工进展 ›› 2024, Vol. 43 ›› Issue (5): 2760-2775.DOI: 10.16085/j.issn.1000-6613.2024-0098
• 二氧化碳捕集与资源化利用 • 上一篇
黄澎1(), 邹颖2, 王宝焕2, 王逍妍2, 赵勇1, 梁鑫2(
), 胡迪1
收稿日期:
2024-01-14
修回日期:
2024-04-25
出版日期:
2024-05-15
发布日期:
2024-06-15
通讯作者:
梁鑫
作者简介:
黄澎(1982—),男,博士,研究员,研究方向为煤炭洁净转化、固废利用、CO2还原和精细化学品等。E-mail:squallok@qq.com。
基金资助:
HUANG Peng1(), ZOU Ying2, WANG Baohuan2, WANG Xiaoyan2, ZHAO Yong1, LAING Xin2(
), HU Di1
Received:
2024-01-14
Revised:
2024-04-25
Online:
2024-05-15
Published:
2024-06-15
Contact:
LAING Xin
摘要:
利用电催化二氧化碳还原反应(CRR)将CO2转变为有价值的合成气(CO/H2)受到广泛关注。CRR电催化剂的开发对于高效、精确制备合成气至关重要。本文综述了CRR制备合成气的反应过程、反应机理以及催化剂等方面的研究进展,介绍了现有CRR催化剂的种类、优点、存在的问题以及发展方向,具体分析了催化剂的掺杂元素种类和比例对反应中间体的影响,指出了掺杂非金属元素的金属原子边缘和活性位对CRR的作用,探讨了催化剂设计和反应条件调节对CO和H2比例的精确调控。本文也讨论了增加反应活性位点、降低中间体的反应能垒等促进CRR以及调节合成气碳氢比的方式。此外,提出了可通过催化剂多级形貌调控、多活性位点设计、CO2还原与阳极反应耦合等途径,提升CRR制合成气效率的策略。最后,探讨和展望了CRR制合成气在未来工业化生产中存在的挑战和问题。
中图分类号:
黄澎, 邹颖, 王宝焕, 王逍妍, 赵勇, 梁鑫, 胡迪. 二氧化碳电催化还原反应制合成气催化剂研究进展[J]. 化工进展, 2024, 43(5): 2760-2775.
HUANG Peng, ZOU Ying, WANG Baohuan, WANG Xiaoyan, ZHAO Yong, LAING Xin, HU Di. Research progress of electrocatalysts towards electrocatalytic reduction reaction of carbon dioxide to syngas[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2760-2775.
电化学半反应 | 电极电位(vs. SHE)/ V |
---|---|
2H+ + 2e- | -0.420 |
CO2 (g) + 2H+ + 2e- | -0.250 |
CO2 (g) + H2O (l) + e- | -1.078 |
CO2 (g) + 2H+ + 2e- | -0.106 |
CO2 (g) + H2O (l) + 2e- | -0.934 |
表1 在标准大气压和25℃下,部分CRR产物及其在中性水溶液中相对标准氢电极(SHE)的平衡电势[16]
电化学半反应 | 电极电位(vs. SHE)/ V |
---|---|
2H+ + 2e- | -0.420 |
CO2 (g) + 2H+ + 2e- | -0.250 |
CO2 (g) + H2O (l) + e- | -1.078 |
CO2 (g) + 2H+ + 2e- | -0.106 |
CO2 (g) + H2O (l) + 2e- | -0.934 |
催化剂名称 | 过电位(vs. RHE)/V | 电流密度/mA·cm-2 | 电解质 | 法拉第效率/% | 参考文献 |
---|---|---|---|---|---|
Fe3+-N-C | -0.45 | 15 | 0.5mol/L KHCO3 | 90 | [ |
Mn-NO/CNs | -0.46 | 8 | 0.5mol/L KHCO3 | 96 | [ |
Ni-N4-C | -0.4 | 8 | 0.5mol/L KHCO3 | 90.2 | [ |
P/Ni-0@Ni-N-C | -0.8 | 20 | 0.5mol/L KHCO3 | 91 | [ |
ZnN/CNO | -0.47 | 5.5 | 0.5mol/L KHCO3 | 97 | [ |
Fe1-Ni1-N-C | -0.5 | 7 | 0.5mol/L KHCO3 | 96.2 | [ |
Au NWs | -0.35 | 8 | 0.5mol/L KHCO3 | 94 | [ |
DDT-Au | -1.1 | 2.4 | 0.1mol/L KHCO3+3.4μmol/L EDTA | 40 | [ |
ID-Ag | -0.7 | 18 | 0.5mol/L KHCO3 | 94.5 | [ |
Ag | -0.49 | 3 | 0.1mol/L KHCO3 | 80 | [ |
AuCu/CNT | -0.4 | 2 | 0.5mol/L KHCO3 | 95.2 | [ |
Cu/Ni(OH)2 | -0.39 | 4.3 | 0.5mol/L NaHCO3 | 92 | [ |
ZnCa-MOF74 | -1.9V (vs.SCE) | 4 | 0.1mol/L KHCO3 | 93 | [ |
Zn x Cd1-x @S-胺 | -1.16 | 25 | 0.5mol/L NaHCO3 | 60 | [ |
p-Cu@Zn(101) | -0.39 | 11.36 | 0.1mol/L KHCO3 | 85 | [ |
FeNPCN | -0.5 | 3 | 0.1mol/L KHCO3 | 94 | [ |
Ni SAs/NCNTs | -0.75 | 22 | 0.5mol/L KHCO3 | 95 | [ |
CoPc/CNT | -0.52 | 15 | 0.1mol/L KHCO3 | 96 | [ |
NC-900 | -0.35 | 5 | 0.5mol/L NaHCO3 | 90 | [ |
1D/2D NR/CS-900 | -0.45 | 16 | 0.5mol/L KHCO3 | 94.2 | [ |
NSHPC | -0.6 | 5.58 | 0.1mol/L KHCO3 | 87.8 | [ |
SD-AgPMRs | -0.38 | 2.3 | 0.1mol/L KHCO3 | 80 | [ |
NP-C | -0.59 | 5.5 | 0.1mol/L KHCO3 | 81 | [ |
BPNC | -0.5 | 3 | 0.1mol/L KHCO3 | 81.8 | [ |
表2 文中催化剂汇总
催化剂名称 | 过电位(vs. RHE)/V | 电流密度/mA·cm-2 | 电解质 | 法拉第效率/% | 参考文献 |
---|---|---|---|---|---|
Fe3+-N-C | -0.45 | 15 | 0.5mol/L KHCO3 | 90 | [ |
Mn-NO/CNs | -0.46 | 8 | 0.5mol/L KHCO3 | 96 | [ |
Ni-N4-C | -0.4 | 8 | 0.5mol/L KHCO3 | 90.2 | [ |
P/Ni-0@Ni-N-C | -0.8 | 20 | 0.5mol/L KHCO3 | 91 | [ |
ZnN/CNO | -0.47 | 5.5 | 0.5mol/L KHCO3 | 97 | [ |
Fe1-Ni1-N-C | -0.5 | 7 | 0.5mol/L KHCO3 | 96.2 | [ |
Au NWs | -0.35 | 8 | 0.5mol/L KHCO3 | 94 | [ |
DDT-Au | -1.1 | 2.4 | 0.1mol/L KHCO3+3.4μmol/L EDTA | 40 | [ |
ID-Ag | -0.7 | 18 | 0.5mol/L KHCO3 | 94.5 | [ |
Ag | -0.49 | 3 | 0.1mol/L KHCO3 | 80 | [ |
AuCu/CNT | -0.4 | 2 | 0.5mol/L KHCO3 | 95.2 | [ |
Cu/Ni(OH)2 | -0.39 | 4.3 | 0.5mol/L NaHCO3 | 92 | [ |
ZnCa-MOF74 | -1.9V (vs.SCE) | 4 | 0.1mol/L KHCO3 | 93 | [ |
Zn x Cd1-x @S-胺 | -1.16 | 25 | 0.5mol/L NaHCO3 | 60 | [ |
p-Cu@Zn(101) | -0.39 | 11.36 | 0.1mol/L KHCO3 | 85 | [ |
FeNPCN | -0.5 | 3 | 0.1mol/L KHCO3 | 94 | [ |
Ni SAs/NCNTs | -0.75 | 22 | 0.5mol/L KHCO3 | 95 | [ |
CoPc/CNT | -0.52 | 15 | 0.1mol/L KHCO3 | 96 | [ |
NC-900 | -0.35 | 5 | 0.5mol/L NaHCO3 | 90 | [ |
1D/2D NR/CS-900 | -0.45 | 16 | 0.5mol/L KHCO3 | 94.2 | [ |
NSHPC | -0.6 | 5.58 | 0.1mol/L KHCO3 | 87.8 | [ |
SD-AgPMRs | -0.38 | 2.3 | 0.1mol/L KHCO3 | 80 | [ |
NP-C | -0.59 | 5.5 | 0.1mol/L KHCO3 | 81 | [ |
BPNC | -0.5 | 3 | 0.1mol/L KHCO3 | 81.8 | [ |
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