Covalent Organic Framework Materials for Photo/ Electrocatalytic Carbon Dioxide Reduction

doi:10.19894/j.issn.1000-0518.210439

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (4): 559-584.DOI: 10.19894/j.issn.1000-0518.210439

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Covalent Organic Framework Materials for Photo/ Electrocatalytic Carbon Dioxide Reduction

Lin-Jie SHANG¹, Jiang LIU¹(), Ya-Qian LAN²()

^1.School of Chemistry and Materials Science，Nanjing Normal University，Nanjing 210023，China
^2.School of Chemistry，South China Normal University，Guangzhou 510006，China

Received:2021-08-30 Accepted:2021-11-24 Published:2022-04-01 Online:2022-04-19
Contact: Jiang LIU,Ya-Qian LAN
Supported by:
the National Natural Science Foundation of China(21871141)

Abstract

Abstract:

Covalent organic frameworks （COFs） are a class of emerging materials connected by covalent bonds， which have high thermal/chemical stability （except boric acid COFs）， permanent porosity， large specific surface area and good crystallinity. In addition， the structure of the monomer unit in COFs is adjustable and can coordinate with many transition metal ions to provide catalytic active sites. These advantages make COFs helpful to catalyze various reactions. Among them， COFs have an excellent catalytic effect on the CO₂ reduction reaction （CO₂RR）. This is mainly because the adjustable pore structure of COFs allows them to adsorb a large amount of CO₂ and the π-π stacking structure in COFs can promote charge transfer， which can greatly improve the efficiency of CO₂ reduction. COFs can be used as photo/electrocatalysts to efficiently reduce CO₂ to CO， CH₄， HCOOH and other products. This review discusses the important achievements of CO₂RR catalyzed by COFs， including photo/electrocatalytic CO₂RR and photoelectric coupling CO₂RR. In addition， the future development of COFs as CO₂RR catalysts is also prospected.

Key words: Covalent organic frameworks, Photocatalysis, Electrocatalysis, Carbon dioxide reduction

CLC Number:

O622

Lin-Jie SHANG, Jiang LIU, Ya-Qian LAN. Covalent Organic Framework Materials for Photo/ Electrocatalytic Carbon Dioxide Reduction[J]. Chinese Journal of Applied Chemistry, 2022, 39(4): 559-584.

Figures/Tables 32

Table 1 The main products of CO2 reduction in H2O and the corresponding reduction potentials

序号 No.	化学反应 Chemical reactions	氧化还原电势/V（vs NHE） Oxidation?reduction potential/V（vs NHE）
（1）	CO₂+2H⁺ +2e^- → CO+H₂O	-0.53
（2）	CO₂+2H⁺+2e^- → HCOOH	-0.61
（3）	CO₂+4H⁺+4e^- → HCHO+H₂O	-0.48
（4）	CO₂+4H⁺+4e^- → C+2H₂O	-0.20
（5）	CO₂+6H⁺+6e^- → CH₃OH+H₂O	-0.38
（6）	CO₂+8H⁺+8e^- → CH₄+2H₂O	-0.24
（7）	2CO₂ + 12H⁺+12e^- → C₂H₅OH+3H₂O	-0.33
（8）	2CO₂+12H⁺+12e^- → C₂H₄+4H₂O	-0.34
（9）	2CO₂+14H⁺+14e^- → C₂H₆+4H₂O	-0.27
（10）	3CO₂+18H⁺+18e^- → C₃H₇OH+5H₂O	-0.32

Fig.1 Schematic illustration of the COF film photocatalyst-enzyme coupled system［40］

Fig.2 Schematic of the mechanism of TTCOF-M CO2RR with H2O oxidation［44］

Fig.3 The photocatalytic conversion of CO2 into CO over COF-367-Co NSs under visible-light irradiation with ［Ru（bpy）3］2+ as the photosensitizer and AA as the electron donor［45］

Fig.4 Rational fabrication of COF-367-Co featuring different spin states of Co ions toward photocatalytic CO2 reduction［46］

Fig.5 Photocatalytic selective reduction of CO2 over Ni-TpBpy COF［47］

Fig.6 Catalytic mechanism for CO2 reduction over Re-COF［48］

Fig.7 Synthesis of CTF-py and Re-CTF-py materials. The inset shows the two types of pores （unit A and unit B）［49］

Fig.8 Proposed mechanisms for photocatalytic reduction of CO2 with DQTP COF-M［51］

Fig.9 Schematic illustration of the possible photocatalytic reduction of CO2 to CO mechanism over Co/CTF-1 under visible light［53］

Fig.10 Proposed mechanism for the photochemical reaction comprising an electron transfer relay process with Por-CTF as the relay facilitator for carbon dioxide reduction in a ternary hybrid system［54］

Fig.11 Schematic representation of the preparation of COF-318-SCs via the condensation of COF-318 and semiconductor materials［55］

Fig.12 Synthesis route of TAPBB-COF［56］

Fig.13 Proposed photoactive electron transfer and reaction pathway in the photoreduction of CO2 （PET=photoinduced electron transfer）［57］

Fig.14 The CO2 reduction inferential path of COF-TVBT-PA［58］Carbon （grey）， nitrogen （blue）， oxygen （red） and hydrogen （white）

Fig.15 Possible reaction mechanism for photocatalytic reduction of CO2 over 2D CN-COF［59］

Fig.16 Schematic diagram for the photocatalytic reduction of CO2 over TpBD-X ［X=—H2， —（CH3）2， —（OCH3）2 and —（NO2）2］ upon visible-light irradiation［60］

Fig.17 An illustration showing the Ni sites in Ni-CTF （weakly adsorbed molecules in electrolyte， such as water and ethanol used for the preparation of electrode， are not shown for clarity）［62］

Fig.18 Schematic representation of the preparation of Cu/ICTF and its transformation in CO2RR conditions： CO2-saturated electrolyte containing a KHCO3 （0.1 mol/L） and KCl （0.1 mol/L） solution［63］

Fig.19 Four CO2RR catalytic mechanisms to form CO （Paths 1－4）［64］

Fig.20 Proposed mechanism for electrocatalytic CO2 reduction in COF-366-Co［66］

Fig.21 Synthesis of NiPor-CTF through ionothermal strategy［67］

Fig.22 The proposed diagram of FeDhaTph-COF in CO2RR［68］

Fig.23 Schematic diagram for the construction of the COF-Based catalysts with isolated cobalt porphyrin units［69］

Fig.24 Atomic structure of the COF series and the corresponding fragments［72］

Fig.25 Schematic illustration for the synthesis of 2D conductive NiPc-COF with top view and side view of the slipped AA stacking structure［73］

Fig.26 The synthesis of COF-2，2′-bpy-Re from COF-2，2′-bpy［75］

Fig.27 The schematic diagram of COF-Re_M in CO2RR［77］

Fig.28 Schematic diagram of BAC-COFs structure （the inset in the upper right corner is a “M1/M2-N6” catalytic unit）［78］The black， blue， green， yellow and pink colors represent C， N， H， M1 and M2， respectively

Fig.29 Scheme for COF-300 reduction［79］

Fig.30 Reaction scheme and the structure of FN-CTF-400［80］

Fig.31 Schematic of the synthesis and structure of MPc-TFPN COF through the condensation of MPc-8OH and TFPN［82］

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Covalent Organic Framework Materials for Photo/ Electrocatalytic Carbon Dioxide Reduction

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