The functionality of surface hydroxyls on selective CH<sub>4</sub> generation from photoreduction of CO<sub>2</sub> over SiC nanosheets

Han, Cheng; Lei, Yongpeng; Wang, Bing; Wu, Chunzhi; Zhang, Xiaoshan; Shen, Shujin; Sun, Lian; Tian, Qiong; Feng, Qingguo; Wang, Kunjie

doi:10.1039/c8cc09371g

Cited by 19 publications

(17 citation statements)

References 44 publications

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“…Our DFT calculations also have shown that the binding of CO* with the P atoms becomes stronger after the incorporation of CTF with BP, leading to the high CH 4 selectivity from CO* hydrogenation . In addition, the improved CH 4 selectivity of CTF-BP catalysts can be attributed to the collaborative effects of enhanced reduction potential, concentrated electron density, and pronounced charge transfer . All of these factors explain why the improved CH 4 selectivity of CTF-BP catalysts is observed in this work.…”

Section: Resultssupporting

confidence: 61%

“…Furthermore, DFT-calculated binding energies of CO* over the P atom of the 2D/2D CTF-BP heterostructure and the pure 2D BP catalysts are −38 and −16 kJ/mol, respectively, indicating that the CO* binding with P atoms becomes stronger after the incorporation of CTF with BP. This enhances the further hydrogenation of CO* to CH 4 resulting in the higher selectivity of CH 4 for the CTF-BP heterostructured catalyst . Compared with the pristine CTF, a better photocatalytic performance is achieved.…”

Section: Resultsmentioning

confidence: 99%

“…This enhances the further hydrogenation of CO* to CH 4 resulting in the higher selectivity of CH 4 for the CTF-BP heterostructured catalyst. 46 Compared with the pristine CTF, a better photocatalytic performance is achieved. Based on these electronic structure calculations of charge distributions, the generation, separation, migration, and reaction of holes and electrons can be illustrated.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…50 In addition, the improved CH 4 selectivity of CTF-BP catalysts can be attributed to the collaborative effects of enhanced reduction potential, 51 concentrated electron density, 52 and pronounced charge transfer. 46…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO₂ Photoreduction

Liu

Huang

et al. 2020

ACS Sustainable Chem. Eng.

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Photoreduction of CO 2 to CH 4 , which is an 8-electron photoelectrochemical process, represents one of the most appealing approaches that tackles the global warming challenge and fuel crisis. To achieve this, highly efficient and selective catalysts are desired. In this work, we successfully developed a metal-free 2D/2D heterostructured catalyst for photoreduction of CO 2 to CH 4 with black phosphorus (BP) and covalent triazine framework (CTF). The synthesized CTF-BP heterostructure catalyst was well characterized using the high-resolution TEM (HRTEM), AFM, XPS and Raman. Compared with the pristine BP or CTF, the photoreduction of CO 2 to CO rate over the CTF-BP catalyst (4.60 μmol g −1 h −1 ) is 3 and 2 times higher than those over BP and CTF catalysts, respectively. The photoreduction of CO 2 to CH 4 rate over the CTF-BP catalyst (7.81 μmol g −1 h −1 ) is 23 times and 16 times higher than those over BP and CTF catalysts, respectively. This indicates that the CTF-BP heterostructure dramatically enhances the photocatalytic selectivity for CO 2 to CH 4 over CO. The present work not only develops a metal-free highly efficient and selective catalyst for photoreduction of CO 2 but also provides a new heterostructure engineering route for designing and synthesizing highly active and metal-free catalysts applied in sustainable solar-to-chemical energy conversion and environmental remediation.

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Section: Resultssupporting

confidence: 61%

Section: Resultsmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

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Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO₂ Photoreduction

Liu

Huang

et al. 2020

ACS Sustainable Chem. Eng.

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“…Moreover, the enhanced CH 4 selectivity of heterojunction CTF-BP materials can be ascribed to the collaborative effects of improved photocatalytic CO 2 reduction potential, [252] concentrated electron density, [253] and pronounced charge transfer. [254] Although the BP materials can be used as photocatalysts to improve the photocatalytic performance of CO 2 reduction, but the actual reaction active sites for CO 2 reduction of BP still need to be explored in the further experiment.…”

Section: Reaction Mechanism Of Bp-based Photocatalystsmentioning

confidence: 99%

A Critical Review on Black Phosphorus‐Based Photocatalytic CO₂ Reduction Application

Zhao

Long

et al. 2021

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Comparative Studies of Oxygen‐Free Semiconductors in Photocatalytic CO₂ Reduction and Alcohol Degradation

Lorenz

Moustakas

Peppel

et al. 2022

Chemie Ingenieur Technik

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Commercially available a-SiC, b-SiC, GaN, ZnTe and self-synthesized g-C 3 N 4 were investigated in a comparative study regarding their photocatalytic capabilities in CO 2 reduction and alcohol degradation. Under reproducible high-purity solid-gas conditions none of the tested materials promoted CO 2 reduction using H 2 O as proton donor, although TiO 2 P25 has been shown to produce significant amounts of CH 4 under similar conditions. Replacing H 2 O with 2-propanol led to hydrocarbon formation which could solely be attributed to alcohol degradation while no CO 2 reduction took place.

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The functionality of surface hydroxyls on selective CH₄ generation from photoreduction of CO₂ over SiC nanosheets

Abstract: The hydroxyls on SiC nanosheet provide local protons, stabilize the intermediates and localize the electrons for deep photoreduction of CO2.

Cited by 19 publications

References 44 publications

Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO₂ Photoreduction

Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO₂ Photoreduction

A Critical Review on Black Phosphorus‐Based Photocatalytic CO₂ Reduction Application

Comparative Studies of Oxygen‐Free Semiconductors in Photocatalytic CO₂ Reduction and Alcohol Degradation

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The functionality of surface hydroxyls on selective CH4 generation from photoreduction of CO2 over SiC nanosheets

Abstract: The hydroxyls on SiC nanosheet provide local protons, stabilize the intermediates and localize the electrons for deep photoreduction of CO2.

Cited by 19 publications

References 44 publications

Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO2 Photoreduction

Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO2 Photoreduction

A Critical Review on Black Phosphorus‐Based Photocatalytic CO2 Reduction Application

Comparative Studies of Oxygen‐Free Semiconductors in Photocatalytic CO2 Reduction and Alcohol Degradation

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Resources

About

The functionality of surface hydroxyls on selective CH₄ generation from photoreduction of CO₂ over SiC nanosheets

Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO₂ Photoreduction

Metal-Free 2D/2D Black Phosphorus and Covalent Triazine Framework Heterostructure for CO₂ Photoreduction

A Critical Review on Black Phosphorus‐Based Photocatalytic CO₂ Reduction Application

Comparative Studies of Oxygen‐Free Semiconductors in Photocatalytic CO₂ Reduction and Alcohol Degradation