Defect engineering of photocatalysts towards elevated CO2 reduction performance

ChemSusChem ◽  
2021 ◽  
Author(s):  
Meng Shen ◽  
Lingxia Zhang ◽  
Jianlin Shi
Keyword(s):  
Elevated Co2 ◽  
Co2 Reduction ◽  
Defect Engineering

scholarly journals Improving the Catalytic CO2 Reduction on Cs2AgBiBr6 by Halide Defect Engineering: A DFT Study

Materials ◽  
2021 ◽  
Vol 14 (10) ◽  
pp. 2469
Author(s):  
Pengfei Chen ◽  
Yiao Huang ◽  
Zuhao Shi ◽  
Xingzhu Chen ◽  
Neng Li
Keyword(s):  
Gas Adsorption ◽  
Catalytic Reduction ◽  
Deep Level ◽  
Critical Role ◽  
Co2 Reduction ◽  
First Principles Calculation ◽  
Bandgap Energy ◽  
Practical Implementation ◽  
Co2 Conversion ◽  
Defect Engineering

Pb-free double halide perovskites have drawn immense attention in the potential photocatalytic application, due to the regulatable bandgap energy and nontoxicity. Herein, we first present a study for CO2 conversion on Pb-free halide perovskite Cs2AgBiBr6 under state-of-the-art first-principles calculation with dispersion correction. Compared with the previous CsPbBr3, the cell parameter of Cs2AgBiBr6 underwent only a small decrease of 3.69%. By investigating the adsorption of CO, CO2, NO, NO2, and catalytic reduction of CO2, we found Cs2AgBiBr6 exhibits modest adsorption ability and unsatisfied potential determining step energy of 2.68 eV in catalysis. We adopted defect engineering (Cl doping, I doping and Br-vacancy) to regulate the adsorption and CO2 reduction behavior. It is found that CO2 molecule can be chemically and preferably adsorbed on Br-vacancy doped Cs2AgBiBr6 with a negative adsorption energy of −1.16 eV. Studying the CO2 reduction paths on pure and defect modified Cs2AgBiBr6, Br-vacancy is proved to play a critical role in decreasing the potential determining step energy to 1.25 eV. Finally, we probe into the electronic properties and demonstrate Br-vacancy will not obviously promote the process of catalysis deactivation, as there is no formation of deep-level electronic states acting as carrier recombination center. Our findings reveal the process of gas adsorption and CO2 reduction on novel Pb-free Cs2AgBiBr6, and propose a potential strategy to improve the efficiency of catalytic CO2 conversion towards practical implementation.

Defect Engineering in Polymeric Cobalt Phthalocyanine Networks for Enhanced Electrochemical CO2 Reduction

2018 ◽  
Vol 5 (19) ◽  
pp. 2717-2721 ◽  
Author(s):  
Haihong Wu ◽  
Min Zeng ◽  
Xiang Zhu ◽  
Chengcheng Tian ◽  
Bingbao Mei ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Cobalt Phthalocyanine ◽  
Defect Engineering ◽  
Electrochemical Co2 Reduction

(Invited) Defect Engineering and Surface Probing of Few-Layer MoS2 As Photocatalyst for CO2 Reduction to Solar Fuels

2020 ◽  
Vol MA2020-01 (39) ◽  
pp. 1748-1748
Author(s):  
Li-Chyong Chen ◽  
Yi-Fan Huang ◽  
Hsiang-Ting Lien ◽  
He-Yun Du ◽  
Yu-Chung Chang ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Solar Fuels ◽  
Defect Engineering

Controlling defects in crystalline carbon nitride to optimize photocatalytic CO2 reduction

2020 ◽  
Vol 56 (42) ◽  
pp. 5641-5644 ◽  
Author(s):  
Han Li ◽  
Bicheng Zhu ◽  
Shaowen Cao ◽  
Jiaguo Yu
Keyword(s):  
Charge Carrier ◽  
Carbon Nitride ◽  
Co2 Reduction ◽  
Defect Engineering ◽  
Carrier Transfer

Defect engineering in crystalline carbon nitride promotes the charge carrier transfer and CO2 adsorption and activation for enhanced CO2 photoreduction.

scholarly journals Ultra-Thin Carbon-Doped Bi2WO6 Nanosheets for Enhanced Photocatalytic CO2 Reduction

2021 ◽  
Author(s):  
Han Li ◽  
Junchao Zhang ◽  
Jiaguo Yu ◽  
Shaowen Cao
Keyword(s):  
Light Absorption ◽  
Active Sites ◽  
Co2 Reduction ◽  
Charge Recombination ◽  
Charge Carriers ◽  
Carbon Doping ◽  
Defect Engineering ◽  
Carbon Doped ◽  
Promising Strategy ◽  
Thin Carbon

AbstractThe photocatalytic reduction of CO2 is a promising strategy to generate chemical fuels. However, this reaction usually suffers from low photoactivity because of insufficient light absorption and rapid charge recombination. Defect engineering has become an effective approach to improve the photocatalytic activity. Herein, ultra-thin (~ 4.1 nm) carbon-doped Bi2WO6 nanosheets were prepared via hydrothermal treatment followed by calcination. The ultra-thin nanosheet structure of the catalyst not only provides more active sites but also shortens the diffusion distance of charge carriers, thereby suppressing charge recombination. Moreover, carbon doping could successfully extend the light absorption range of the catalyst and remarkably promote charge separation, thus inhibiting recombination. As a result, the as-prepared Bi2WO6 photocatalyst with ultra-thin nanosheet structure and carbon doping exhibits enhanced photocatalytic CO2 reduction performance, which is twice that of pristine ultra-thin Bi2WO6 nanosheet. This study highlights the importance of defect engineering in photocatalytic energy conversion and provides new insights for fabricating efficient photocatalysts.

scholarly journals Vacancy-Defect Modulated Pathway of Photoreduction of CO2 on Quaternary Single Atomically Thin AgInP2S6 Sheets toward Boosting Efficient and Selective Production of Value-Added Olefiant Gas

2021 ◽  
Author(s):  
Yong Zhou ◽  
Zhigang Zou ◽  
Wa Gao ◽  
Xiaoyong Wang ◽  
Qing Shen ◽  
...  
Keyword(s):  
Reaction Pathway ◽  
Co2 Reduction ◽  
Value Added ◽  
Catalytic Efficiency ◽  
Atomic Layer ◽  
Major Product ◽  
Vacancy Defect ◽  
Charge Carriers ◽  
Defect Engineering

Abstract The quaternary AgInP2S6 atomic layer with the thickness of ~ 0.70 nm were successfully synthesized through facile ultrasonic exfoliation of the corresponding bulk crystal. The ultrathin sheet exhibits efficiently photocatalytic conversion of CO2 into CO as a major product and minority of CH4 and C2H4 in the presence of water vapor. The sulfur defect engineering on this atomic layer through a H2O2 etch process can excitingly enable to change the CO2 photoreduction reaction pathway to steer dominant generation of ethene (C2H4) important chemical with the yield-based selectivity reaching ~73% and the electron-based selectivity as high as ~89%, and the quantum yield of 0.51% at wavelength of 415 nm. Both DFT calculation and in-situ FTIR demonstrate as the introduction of S vacancies in AgInP2S6 causes the charge accumulation on the Ag atoms near the S vacancies, the exposed Ag sites can thus effectively capture the forming *CO molecules, making the catalyst surface enrich with key reaction intermediates to lower the C-C binding coupling barrier, which facilitates the production of C2H4. Surface photovoltage measurement confirms that atomically ultrathin structure of the exfoliated AgInP2S6 can shorten the transfer distance of charge carriers from the interior onto the surface, thus decrease the recombination in body and improve the catalytic efficiency. This work may provide fresh insights into the design of atomically thin photocatalyst framework for CO2 reduction and establish an ideal platform for reaffirming the versatility of defect engineering in tuning catalytic activity and selectivity.

Defect-engineering of tin oxide via (Cu, N) co-doping for electrocatalytic and photocatalytic CO2 reduction into formate

2020 ◽  
Vol 227 ◽  
pp. 115947
Author(s):  
Huimin Yang ◽  
Yupeng Li ◽  
Dingding Zhang ◽  
Zhifang Li ◽  
Jiaxin Wang ◽  
...  
Keyword(s):  
Tin Oxide ◽  
Co2 Reduction ◽  
Defect Engineering ◽  
Co Doping

The Plains CO2 Reduction (PCOR) Partnership: CO2 Sequestration Demonstration Projects Adding Value to the Oil and Gas Industry

2013 ◽  
Author(s):  
Charles D. Gorecki ◽  
Edward N. Steadman ◽  
John A. Harju ◽  
James A. Sorensen ◽  
John A. Hamling ◽  
...  
Keyword(s):  
Co2 Sequestration ◽  
Oil And Gas ◽  
Co2 Reduction ◽  
Oil And Gas Industry ◽  
Gas Industry

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.

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