Modulating intramolecular electron and proton transfer kinetics for promoting carbon dioxide conversion

2022 ◽  
Author(s):  
Yajie Yuan ◽  
Yazhen Zhao ◽  
Shuai Yang ◽  
Sheng Han ◽  
Chenbao Lu ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Dipole Moment ◽  
Proton Transfer ◽  
Co2 Reduction ◽  
Iron Porphyrin ◽  
Carbon Dioxide Conversion ◽  
Reduction Activity

A novel pentagon-heptagon paired azulene group which possesses large dipole moment is immobilized to porphyrin. The as–prepared azulene iron porphyrin exhibits narrower bandgap and higher electrocatalytic CO2 reduction activity than...

An NADH-Inspired Redox Mediator Strategy to Promote Second-Sphere Electron and Proton Transfer for Cooperative Electrochemical CO2 Reduction Catalyzed by Iron Porphyrin

2020 ◽  
Author(s):  
Peter T. Smith ◽  
Sophia Weng ◽  
Christopher Chang
Keyword(s):  
Proton Transfer ◽  
Co2 Reduction ◽  
Iron Porphyrin ◽  
Redox Mediators ◽  
Reservoir Properties ◽  
Proton Reduction ◽  
Electrochemical Co2 Reduction ◽  
Starting Point ◽  
Rate Improvement ◽  
Molecular Catalysts

We present a bioinspired strategy for enhancing electrochemical carbon dioxide reduction catalysis by cooperative use of base-metal molecular catalysts with intermolecular second-sphere redox mediators that facilitate both electron and proton transfer. Functional synthetic mimics of the biological redox cofactor NADH, which are electrochemically stable and are capable of mediating both electron and proton transfer, can enhance the activity of an iron porphyrin catalyst for electrochemical reduction of CO<sub>2</sub> to CO, achieving a 13-fold rate improvement without altering the intrinsic high selectivity of this catalyst platform for CO<sub>2</sub> versus proton reduction. Evaluation of a systematic series of NADH analogs and redox-inactive control additives with varying proton and electron reservoir properties reveals that both electron and proton transfer contribute to the observed catalytic enhancements. This work establishes that second-sphere dual control of electron and proton inventories is a viable design strategy for developing more effective electrocatalysts for CO<sub>2</sub> reduction, providing a starting point for broader applications of this approach to other multi-electron, multi-proton transformations.

Direct Z-scheme Sn-In2O3/In2S3 heterojunction nanostructures for enhanced photocatalytic CO2 reduction activity

2021 ◽  
Author(s):  
Yinyi Ma ◽  
Zemin Zhang ◽  
Xiao Jiang ◽  
Rongke Sun ◽  
Mingzheng Xie ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Environmental Pollution ◽  
Light Absorption ◽  
Co2 Reduction ◽  
Photocatalytic Reduction ◽  
Practical Significance ◽  
Energy Crisis ◽  
Low Light ◽  
Reduction Activity

Photocatalytic reduction of carbon dioxide into chemical fuels has great practical significance in solving energy crisis and environmental pollution, but remains a big challenge owing to its low light absorption...

scholarly journals Microwave-Assisted Solvothermal Synthesis of Chalcogenide Composite Photocatalyst and Its Photocatalytic CO2 Reduction Activity under Simulated Solar Light

Catalysts ◽  
2020 ◽  
Vol 10 (7) ◽  
pp. 789
Author(s):  
Gang-Juan Lee ◽  
Yu-Hong Hou ◽  
Hsin-Ting Huang ◽  
Wenmin Wang ◽  
Cong Lyu ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Photocatalytic Activity ◽  
Co2 Reduction ◽  
Carbon Dioxide Reduction ◽  
Photoluminescence Intensity ◽  
Composite Photocatalyst ◽  
Microwave Assisted ◽  
Reduction Activity ◽  
Operation Conditions ◽  
Co Doped

A novel heterostructure consisting of Ru and Cu co-doped ZnS nanopowders (RCZS) into a MoS2-graphene hybrid (MSG) is successfully prepared by the microwave-assisted solvothermal approach. RCZS nanopowders are fabricated on the surface of MSG, which produces a nanoscale interfacial between RCZS and MSG. As the photo-excited electrons of RCZS can easily migrate to MoS2 through graphene by hindering the electron and hole (e– and h+) recombination, the photocatalytic activity could be improved by effective charge transfer. As RCZS are anchored onto the MSG, the photoluminescence intensity of the chalcogenide composite photocatalyst obviously decreases. In addition, a quaternary ruthenium and copper-based chalcogenide RCZS/MSG is able to improve the harvest and utilization of light. With the increase in the concentrations of Ru until 4 mol%, the band gap significantly decreases from 3.52 to 2.73 eV. At the same time, moderate modification by ruthenium can decrease the PL intensity compared to the pristine CZS/MSG sample, which indicates the enhancement of e– and h+ separation by Ru addition. The photocatalytic activity of as-synthesized chalcogenide composite photocatalysts is evaluated by the photocatalytic carbon dioxide reduction. Optimized operation conditions for carbon dioxide reduction have been performed, including the concentration of NaOH solution, the amount of RCZS/MSG photocatalyst, and the content of co-doped ruthenium. The doping of ruthenium would efficiently improve the performance of the photocatalytic activity for carbon dioxide reduction. The optimal conditions, such as the concentration of 2 M NaOH and the 0.5RCZS/MSG dosage of 0.05 g L–1, provide the maximum methane gas yield of 58.6 μmol h−1 g–1.

A highly efficient diatomic nickel electrocatalyst for CO2 reduction

2020 ◽  
Vol 56 (62) ◽  
pp. 8798-8801 ◽  
Author(s):  
Meng-Jiao Sun ◽  
Zhi-Wei Gong ◽  
Jun-Dong Yi ◽  
Teng Zhang ◽  
Xiaodong Chen ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Co2 Reduction ◽  
Carbon Dioxide Reduction ◽  
Carbon Composite ◽  
Nitrogen Doped ◽  
Highly Efficient ◽  
Reduction Activity ◽  
Nitrogen Doped Carbon

Diatomic Ni2 clusters embedded in a nitrogen-doped carbon composite show high electrocatalytic carbon dioxide reduction activity.

An NADH-Inspired Redox Mediator Strategy to Promote Second-Sphere Electron and Proton Transfer for Cooperative Electrochemical CO2 Reduction Catalyzed by Iron Porphyrin

2020 ◽  
Author(s):  
Peter T. Smith ◽  
Sophia Weng ◽  
Christopher Chang
Keyword(s):  
Proton Transfer ◽  
Co2 Reduction ◽  
Iron Porphyrin ◽  
Redox Mediators ◽  
Reservoir Properties ◽  
Proton Reduction ◽  
Electrochemical Co2 Reduction ◽  
Starting Point ◽  
Rate Improvement ◽  
Molecular Catalysts

We present a bioinspired strategy for enhancing electrochemical carbon dioxide reduction catalysis by cooperative use of base-metal molecular catalysts with intermolecular second-sphere redox mediators that facilitate both electron and proton transfer. Functional synthetic mimics of the biological redox cofactor NADH, which are electrochemically stable and are capable of mediating both electron and proton transfer, can enhance the activity of an iron porphyrin catalyst for electrochemical reduction of CO<sub>2</sub> to CO, achieving a 13-fold rate improvement without altering the intrinsic high selectivity of this catalyst platform for CO<sub>2</sub> versus proton reduction. Evaluation of a systematic series of NADH analogs and redox-inactive control additives with varying proton and electron reservoir properties reveals that both electron and proton transfer contribute to the observed catalytic enhancements. This work establishes that second-sphere dual control of electron and proton inventories is a viable design strategy for developing more effective electrocatalysts for CO<sub>2</sub> reduction, providing a starting point for broader applications of this approach to other multi-electron, multi-proton transformations.

scholarly journals Carbon Dioxide Conversion: Tailoring CO2 Reduction with Doped Silicon Nanocrystals (Adv. Sustainable Syst. 11/2017)

2017 ◽  
Vol 1 (11) ◽  
Author(s):  
Annabelle P. Y. Wong ◽  
Wei Sun ◽  
Chenxi Qian ◽  
Abdinoor A. Jelle ◽  
Jia Jia ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Silicon Nanocrystals ◽  
Co2 Reduction ◽  
Carbon Dioxide Conversion ◽  
Doped Silicon

scholarly journals A Comparison of Different Approaches to the Conversion of Carbon Dioxide into Useful Products: Part II : More routes to CO2 reduction

2021 ◽  
Vol 65 (2) ◽  
pp. 197-206
Author(s):  
Annette Alcasabas ◽  
Peter R. Ellis ◽  
Iain Malone ◽  
Gareth Williams ◽  
Chris Zalitis
Keyword(s):  
Carbon Dioxide ◽  
Co2 Reduction ◽  
Current Status ◽  
Future Research ◽  
Research Needs ◽  
Carbon Dioxide Conversion ◽  
Technological Options

In this review, we consider a range of different technological approaches to carbon dioxide conversion, their current status and the molecules which each approach is best suited to making. Part II presents the photochemical, photoelectrochemical, plasma and microbial electrosynthetic routes to CO2 reduction and discusses the technological options together with proposals for future research needs from an industry perspective.

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