化工学报 ›› 2023, Vol. 74 ›› Issue (1): 29-44.DOI: 10.11949/0438-1157.20221120
收稿日期:
2022-08-08
修回日期:
2022-11-04
出版日期:
2023-01-05
发布日期:
2023-03-20
通讯作者:
郭烈锦
作者简介:
王峰(1990—),男,博士研究生,f_wang@xjtu.edu.cn
基金资助:
Feng WANG(), Shunxin ZHANG, Fangbo YU, Ya LIU, Liejin GUO()
Received:
2022-08-08
Revised:
2022-11-04
Online:
2023-01-05
Published:
2023-03-20
Contact:
Liejin GUO
摘要:
光催化CO2还原制碳氢燃料技术由太阳能直接驱动,将CO2转化为可直接利用的化学品,是助力碳达峰、碳中和的变革性技术。该技术的高效、低成本运行受光吸收利用、光催化剂形貌结构、界面催化反应及传质等因素影响,其内部能质传输是多时空尺度、多物理场耦合的复杂过程,需要从理论和应用两方面结合多个学科展开系统研究。梳理了光催化CO2还原基本理论及国内外研究进展,并针对技术瓶颈从光吸收拓展与利用、光生载流子分离强化、氧化/还原半反应优化及传质强化四个优化策略指出了该技术发展方向,探讨了该技术全流程能量传递和物质转化之间的耦合匹配准则,为降低反应能耗、促进性能及产率提升甚至未来工业化大规模太阳能驱动CO2还原应用铺垫道路。
中图分类号:
王峰, 张顺鑫, 余方博, 刘亚, 郭烈锦. 光催化CO2还原制碳氢燃料系统优化策略研究[J]. 化工学报, 2023, 74(1): 29-44.
Feng WANG, Shunxin ZHANG, Fangbo YU, Ya LIU, Liejin GUO. Optimization strategy for producing carbon based fuels by photocatalytic CO2 reduction[J]. CIESC Journal, 2023, 74(1): 29-44.
产物 | 反应 | 氧化还原电位(vs NHE)/V |
---|---|---|
O2 | H2O | +0.82 |
H2 | 2H++2e- | -0.41 |
CH4 | CO2+8H++8e- | -0.24 |
C2H6 | 2CO2+14H++14e- | -0.27 |
CO | CO2+2H++2e- | -0.51 |
CH3OH | CO2+6H++6e- | -0.39 |
C2H5OH | 2CO2+12H++12e- | -0.33 |
CH3CH2CH2OH | 3CO2+18H++18e- | -0.31 |
CH3CH(OH)CH3 | 3CO2+18H++18e- | -0.30 |
HCHO | CO2+4H++4e- | -0.55 |
CH3CHO | 2CO2+10H++10e- | -0.36 |
CH3CH2CHO | 3CO2+16H++16e- | -0.32 |
CH3COCH3 | 3CO2+16H++16e- | -0.31 |
HCOOH | CO2+2H++2e- | -0.58 |
CH3COOH | 2CO2+8H++8e- | -0.31 |
表1 CO2还原过程常见产物及其简化的氧化还原方程和pH=7下的氧化还原电位
Table 1 Common products of CO2 reduction and their simplified Redox equations and Redox potentials at pH=7
产物 | 反应 | 氧化还原电位(vs NHE)/V |
---|---|---|
O2 | H2O | +0.82 |
H2 | 2H++2e- | -0.41 |
CH4 | CO2+8H++8e- | -0.24 |
C2H6 | 2CO2+14H++14e- | -0.27 |
CO | CO2+2H++2e- | -0.51 |
CH3OH | CO2+6H++6e- | -0.39 |
C2H5OH | 2CO2+12H++12e- | -0.33 |
CH3CH2CH2OH | 3CO2+18H++18e- | -0.31 |
CH3CH(OH)CH3 | 3CO2+18H++18e- | -0.30 |
HCHO | CO2+4H++4e- | -0.55 |
CH3CHO | 2CO2+10H++10e- | -0.36 |
CH3CH2CHO | 3CO2+16H++16e- | -0.32 |
CH3COCH3 | 3CO2+16H++16e- | -0.31 |
HCOOH | CO2+2H++2e- | -0.58 |
CH3COOH | 2CO2+8H++8e- | -0.31 |
体系 | 催化剂 | 反应体系 | 还原产物 | 氧化产物 | 产率 | 文献 |
---|---|---|---|---|---|---|
无牺牲剂体系 | In4SnS8 | H2O+CO2 | CH4 CO | O2 | 10.70 μl·h-1 9.39 μl·h-1 | [ |
Pt-TiO2 | H2O+CO2 | CH4 | 1361 μmol·g-1·h-1 | [ | ||
SnS2-C | H2O+CO2 | CH3CHO | 96.66 μmol·g-1·h-1 | [ | ||
CdS/Mn2O3/PAA | H2O+CO2 | HCOOH CH3CH2OH H2 | 1392.3 μmol·g-1·h-1 52.2 μmol·g-1·h-1 2766 μmol·g-1·h-1 | [ | ||
In2S3/Bi2MoO6 | H2O+CO2 | CO | 28.54 μmol·g-1·h-1 | [ | ||
CuIn5S8 | H2O+CO2 | CH4 | 8.7 μmol·g-1·h-1 | [ | ||
Cu2O | H2O+CO2 | CH3OH | 1.2 mol·g-1· h-1 | [ | ||
mCD/CN | H2O+CO2 | CH3OH | 13.9 μmol·g-1·h-1 | [ | ||
g-CN-MI-40 | H2O+CO2 | CH3OH | H2O2 | 4.18 mmol·g-1 | [ | |
Ag-MnO x /CaTiO3 | H2O+CO2 | CO | 11.8 μmol·h-1 | [ | ||
牺牲剂体系 | Ni-ZnS | K2CO3+K2SO3 | HCOOH | — | 427.5 μmol·g-1·h-1 | [ |
VZn-3D-ZnIn2S4 | H2O+TEOA | CO | — | 276.7 μmol·g-1·h-1 | [ | |
CdIn2S4/Co3O4 | H2O+TEOA+Co | CO | — | 5300 μmol·g-1·h-1 | [ | |
O-ZnIn2S4 | H2O+TEOA+CH3CN+Co | CO | — | 1680 μmol·g-1·h-1 | [ | |
CdS/TiO2 | H2O+NaHCO3+HCl | CH4 | — | 11.9 mmol·m-2·h-1 | [ | |
CdS/NH2-UiO-66 | H2O+TEOA | CO | — | 87 μmol·g-1·h-1 | [ | |
COF-5/CoAl-LDH | H2O+ acetonitrile | CO | — | 53.08 μmol·g-1·h-1 | [ | |
Cu/Cd0.5Zn0.5S | TEOA+KHCO3(aq) | C2+ | — | 6.54 μmol·h-1 | [ |
表2 近年来光催化CO2还原代表性工作
Table 2 Representative work of photocatalytic CO2 reduction in recent years
体系 | 催化剂 | 反应体系 | 还原产物 | 氧化产物 | 产率 | 文献 |
---|---|---|---|---|---|---|
无牺牲剂体系 | In4SnS8 | H2O+CO2 | CH4 CO | O2 | 10.70 μl·h-1 9.39 μl·h-1 | [ |
Pt-TiO2 | H2O+CO2 | CH4 | 1361 μmol·g-1·h-1 | [ | ||
SnS2-C | H2O+CO2 | CH3CHO | 96.66 μmol·g-1·h-1 | [ | ||
CdS/Mn2O3/PAA | H2O+CO2 | HCOOH CH3CH2OH H2 | 1392.3 μmol·g-1·h-1 52.2 μmol·g-1·h-1 2766 μmol·g-1·h-1 | [ | ||
In2S3/Bi2MoO6 | H2O+CO2 | CO | 28.54 μmol·g-1·h-1 | [ | ||
CuIn5S8 | H2O+CO2 | CH4 | 8.7 μmol·g-1·h-1 | [ | ||
Cu2O | H2O+CO2 | CH3OH | 1.2 mol·g-1· h-1 | [ | ||
mCD/CN | H2O+CO2 | CH3OH | 13.9 μmol·g-1·h-1 | [ | ||
g-CN-MI-40 | H2O+CO2 | CH3OH | H2O2 | 4.18 mmol·g-1 | [ | |
Ag-MnO x /CaTiO3 | H2O+CO2 | CO | 11.8 μmol·h-1 | [ | ||
牺牲剂体系 | Ni-ZnS | K2CO3+K2SO3 | HCOOH | — | 427.5 μmol·g-1·h-1 | [ |
VZn-3D-ZnIn2S4 | H2O+TEOA | CO | — | 276.7 μmol·g-1·h-1 | [ | |
CdIn2S4/Co3O4 | H2O+TEOA+Co | CO | — | 5300 μmol·g-1·h-1 | [ | |
O-ZnIn2S4 | H2O+TEOA+CH3CN+Co | CO | — | 1680 μmol·g-1·h-1 | [ | |
CdS/TiO2 | H2O+NaHCO3+HCl | CH4 | — | 11.9 mmol·m-2·h-1 | [ | |
CdS/NH2-UiO-66 | H2O+TEOA | CO | — | 87 μmol·g-1·h-1 | [ | |
COF-5/CoAl-LDH | H2O+ acetonitrile | CO | — | 53.08 μmol·g-1·h-1 | [ | |
Cu/Cd0.5Zn0.5S | TEOA+KHCO3(aq) | C2+ | — | 6.54 μmol·h-1 | [ |
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