Earth-Abundant Photocatalytic CO2 Reduction by Multielectron Chargeable Cobalt Porphyrin Catalysts: High CO/H2 Selectivity in Water Based on Phase Mismatch in Frontier MO Association

ACS Catalysis ◽  
2021 ◽  
pp. 10436-10449
Author(s):  
Xian Zhang ◽  
Kosei Yamauchi ◽  
Ken Sakai
2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Jeremy L. Hitt ◽  
Yuguang C. Li ◽  
Songsheng Tao ◽  
Zhifei Yan ◽  
Yue Gao ◽  
...  

AbstractIn the problem of electrochemical CO2 reduction, the discovery of earth-abundant, efficient, and selective catalysts is essential to enabling technology that can contribute to a carbon-neutral energy cycle. In this study, we adapt an optical high throughput screening method to study multi-metallic catalysts for CO2 electroreduction. We demonstrate the utility of the method by constructing catalytic activity maps of different alloyed elements and use X-ray scattering analysis by the atomic pair distribution function (PDF) method to gain insight into the structures of the most active compositions. Among combinations of four elements (Au, Ag, Cu, Zn), Au6Ag2Cu2 and Au4Zn3Cu3 were identified as the most active compositions in their respective ternaries. These ternary electrocatalysts were more active than any binary combination, and a ca. 5-fold increase in current density at potentials of −0.4 to −0.8 V vs. RHE was obtained for the best ternary catalysts relative to Au prepared by the same method. Tafel plots of electrochemical data for CO2 reduction and hydrogen evolution indicate that the ternary catalysts, despite their higher surface area, are poorer catalysts for the hydrogen evolution reaction than pure Au. This results in high Faradaic efficiency for CO2 reduction to CO.


Author(s):  
Rajasekaran Elakkiya ◽  
Govindhan Maduraiveeran

Design of high-performance and Earth-abundant electrocatalysts for electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) into fuels and value-added chemicals offers an emergent pathway for environment and energy sustainable concerns. Herein,...


2017 ◽  
Vol 8 (1) ◽  
pp. 458-465 ◽  
Author(s):  
Adrien J. Göttle ◽  
Marc T. M. Koper

We provide a complete and computationally detailed picture of the mechanism of the initial stages of the electrocatalytic reduction of CO2 in water catalysed by cobalt porphyrin complexes.


2020 ◽  
Author(s):  
Wei Tang ◽  
Yunyuan Qiu ◽  
Xiaonan Li ◽  
Rodah C. Soy ◽  
John Mack ◽  
...  

<p>Supporting Information for article. </p> <p>Earth-abundant first row transition metal corrole complexes have played an important role in fundamental research due to their unique molecular structures and attractive properties. In comparison to porphyrins, corroles have three inner N-H protons and are ring-contracted with a smaller macrocyclic cavity. First row transition metal corroles have been widely used as effective electrochemical catalysts for small molecule activations, such as hydrogen evolution, oxygen reduction/evolution and CO2 reduction reactions (HERs, ORRs/OERs and CO2 RRs) through homogenous and/or heterogenous prodecures. Several strategies have been used to modulate the catalytic efficiency of synthetic metallocorroles.</p>


ACS Catalysis ◽  
2016 ◽  
Vol 7 (1) ◽  
pp. 70-88 ◽  
Author(s):  
Hiroyuki Takeda ◽  
Claudio Cometto ◽  
Osamu Ishitani ◽  
Marc Robert

ACS Catalysis ◽  
2019 ◽  
Vol 9 (6) ◽  
pp. 4867-4874 ◽  
Author(s):  
Arnau Call ◽  
Mihaela Cibian ◽  
Keiya Yamamoto ◽  
Takashi Nakazono ◽  
Kosei Yamauchi ◽  
...  

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Kang-Qiang Lu ◽  
Yue-Hua Li ◽  
Fan Zhang ◽  
Ming-Yu Qi ◽  
Xue Chen ◽  
...  

Abstract The performance of transition metal hydroxides, as cocatalysts for CO2 photoreduction, is significantly limited by their inherent weaknesses of poor conductivity and stacked structure. Herein, we report the rational assembly of a series of transition metal hydroxides on graphene to act as a cocatalyst ensemble for efficient CO2 photoreduction. In particular, with the Ru-dye as visible light photosensitizer, hierarchical Ni(OH)2 nanosheet arrays-graphene (Ni(OH)2-GR) composites exhibit superior photoactivity and selectivity, which remarkably surpass other counterparts and most of analogous hybrid photocatalyst system. The origin of such superior performance of Ni(OH)2-GR is attributed to its appropriate synergy on the enhanced adsorption of CO2, increased active sites for CO2 reduction and improved charge carriers separation/transfer. This work is anticipated to spur rationally designing efficient earth-abundant transition metal hydroxides-based cocatalysts on graphene and other two-dimension platforms for artificial reduction of CO2 to solar chemicals and fuels.


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