Selectively triggering photoelectrons for CO2-to-CH4 reduction over {110} SrTiO3 with dual-metal sites

2021 ◽  
Author(s):  
Lei Lu ◽  
Xiaopeng Zhu ◽  
Shaomang Wang ◽  
Taozhu Li ◽  
Shicheng Yan ◽  
...  
Keyword(s):  
Active Sites ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Photocatalytic Efficiency ◽  
The Poor ◽  
Strong Adsorption ◽  
Weak Adsorption ◽  
Adsorption Of Co ◽  
Surface Active ◽  
Dual Metal

Abstract In this article, the roles of surface-active sites in dominating photoelectron selectivity for CO2 reduction products are well demonstrated over photocatalyst models of {100} SrTiO3 and {110} SrTiO3. On the easily exposed {100} facets terminated with Sr-O atoms, photoelectrons are of 8 mol % for CH4 and 92 mol % for CO generation. The Sr-O-Ti configuration in the {110} facets could enrich the surface charge density due to the lower interface resistance for higher photocatalytic efficiency (1.6-fold). The dual sites of Ti and adjacent Sr atoms are active for strong adsorption and activation of the generated CO* species from primary CO2 reduction on the surface, thus kinetically favoring the activity of photoelectrons (73 mol %) in hydrogenation for CH2* species and hence CH4 product. Inversely, the poor CH4 selectivity is due to difficulty in subsequent photoelectron reduction reaction by the weak adsorption of CO* at the single-Sr site on the {100} facets, independent of the electron and proton concentration. Our results may offer some illuminating insights into the design of a highly efficient photocatalyst for selective CO2 reduction.

Atomic regulation of metal-organic framework derived carbon-based single-atom catalysts for electrochemical CO2 reduction reaction

2021 ◽  
Author(s):  
Danni Zhou ◽  
Xinyuan Li ◽  
Huishan Shang ◽  
Fengjuan Qin ◽  
Wenxing Chen
Keyword(s):  
Active Sites ◽  
Metal Organic Framework ◽  
Co2 Reduction ◽  
Carbon Dioxide Reduction ◽  
Reduction Reaction ◽  
Single Atom ◽  
Electrochemical Co2 Reduction ◽  
Metal Organic ◽  
Co2 Reduction Reaction ◽  
Organic Framework

Metal-organic framework (MOF) derived single-atom catalysts (SACs), featured unique active sites and adjustable topological structures, exhibit high electrocatalytic performance on carbon dioxide reduction reactions (CO2RR). By modulating elements and atomic...

Identifying Active Sites of Nitrogen-Doped Carbon Materials for the CO2 Reduction Reaction

2018 ◽  
Vol 28 (21) ◽  
pp. 1800499 ◽  
Author(s):  
Song Liu ◽  
Hongbin Yang ◽  
Xiang Huang ◽  
Linghui Liu ◽  
Weizheng Cai ◽  
...  
Keyword(s):  
Active Sites ◽  
Carbon Materials ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Nitrogen Doped ◽  
Nitrogen Doped Carbon ◽  
Co2 Reduction Reaction

scholarly journals Investigating the Nature of the Active Sites for the CO2 Reduction Reaction on Carbon-Based Electrocatalysts

ACS Catalysis ◽  
2019 ◽  
Vol 9 (9) ◽  
pp. 7668-7678 ◽  
Author(s):  
Tristan Asset ◽  
Samuel T. Garcia ◽  
Sergio Herrera ◽  
Nalin Andersen ◽  
Yechuan Chen ◽  
...  
Keyword(s):  
Active Sites ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Co2 Reduction Reaction ◽  
Carbon Based

Probing the enhanced catalytic activity of carbon nanotube supported Ni-LaOx hybrids for the CO2 reduction reaction

Nanoscale ◽  
2018 ◽  
Vol 10 (29) ◽  
pp. 14207-14219 ◽  
Author(s):  
Jie Gao ◽  
Qian Jiang ◽  
Yuefeng Liu ◽  
Wei Liu ◽  
Wei Chu ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Carbon Nanotube ◽  
Active Sites ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Methane Selectivity ◽  
Co2 Reduction Reaction ◽  
Supported Ni

The promoted active sites for the CO2 reduction reaction on Ni-LaOx/oCNT consist of LaOx species on the surface of Ni NPs and are responsible for the highest TOF rate (51.8 × 10−3 s−1) of CO2 conversion with 100% methane selectivity at 240 °C.

scholarly journals Photoelectrochemical Reduction of CO2 to Syngas by Reduced Ag Catalysts on Si Photocathodes

2020 ◽  
Vol 10 (10) ◽  
pp. 3487 ◽  
Author(s):  
Changyeon Kim ◽  
Seokhoon Choi ◽  
Min-Ju Choi ◽  
Sol A Lee ◽  
Sang Hyun Ahn ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Active Sites ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Hydrogen Electrode ◽  
Faradaic Efficiency ◽  
Onset Potential ◽  
Reduction Of Co2 ◽  
Co2 Reduction Reaction ◽  
Ag Catalysts

The photoelectrochemical reduction of CO2 to syngas that is used for many practical applications has been emerging as a promising technique to relieve the increase of CO2 in the atmosphere. Si has been considered to be one of the most promising materials for photoelectrodes, but the integration of electrocatalysts is essential for the photoelectrochemical reduction of CO2 using Si. We report an enhancement of catalytic activity for CO2 reduction reaction by Ag catalysts of tuned morphology, active sites, and electronic structure through reducing anodic treatment. Our proposed photocathode structure, a SiO2 patterned p-Si photocathode with these reduced Ag catalysts, that was fabricated using electron-beam deposition and electrodeposition methods, provides a low onset-potential of −0.16 V vs. the reversible hydrogen electrode (RHE), a large saturated photocurrent density of −9 mA/cm2 at −1.23 V vs. RHE, and faradaic efficiency for CO of 47% at −0.6 V vs. RHE. This photocathode can produce syngas in the ratio from 1:1 to 1:3, which is an appropriate proportion for practical application. This work presents a new approach for designing photocathodes with a balanced catalytic activity and light absorption to improve the photoelectrochemical application for not only CO2 reduction reaction, but also water splitting or N2 reduction reaction.

scholarly journals Rationally designed transition metal hydroxide nanosheet arrays on graphene for artificial CO2 reduction

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Kang-Qiang Lu ◽  
Yue-Hua Li ◽  
Fan Zhang ◽  
Ming-Yu Qi ◽  
Xue Chen ◽  
...  
Keyword(s):  
Transition Metal ◽  
Active Sites ◽  
Co2 Reduction ◽  
Superior Performance ◽  
Metal Hydroxides ◽  
Nanosheet Arrays ◽  
Earth Abundant ◽  
Adsorption Of Co ◽  
Enhanced Adsorption ◽  
Transition Metal Hydroxides

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.

Subsurface Oxygen Defects Electronically Interacting with Active Sites on In2O3 for Enhanced Photothermocatalytic CO2 Reduction

2021 ◽  
Author(s):  
Weiqin Wei ◽  
Zhen Wei ◽  
Ruizhe Li ◽  
zhenhua Li ◽  
Run Shi ◽  
...  
Keyword(s):  
Active Sites ◽  
Catalyst Surface ◽  
Co2 Reduction ◽  
Catalytic Reactions ◽  
Electronic Coupling ◽  
Turnover Frequency ◽  
Structural Units ◽  
Oxygen Defects ◽  
Subsurface Oxygen ◽  
Surface Active

Abstract Oxygen defects play an important role in many catalytic reactions. Increasing surface oxygen defects can be done through reduction treatment. However, excessive reduction blocks electron channels and deactivates the catalyst surface due to electron-trapped effects by subsurface oxygen defects. How to effectively extract electrons from subsurface oxygen defects which cannot directly interact with reactants is challenging and remains elusive. Herein, we report a metallic In-embedded In2O3 nanoflake catalyst over which the turnover frequency of CO2 reduction into CO increases by a factor of 866 (7615 h-1) and 376 (2990 h-1) at same light intensity and reaction temperature, respectively, compared to In2O3. Under electron-delocalization effect of O-In-(O)Vo-In-In structural units at the interface, the electrons in the subsurface oxygen defects are extracted and gather at surface active sites. This improves the electronic coupling with CO2 and stabilizes COOH intermediate. The study opens up new insights for exquisite electronic manipulation of oxygen defects.

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