Regulating the Metallic Cu–Ga Bond by S Vacancy for Improved Photocatalytic CO2 Reduction to C2H4

Wang, Junyan; Yang, Dao‐Wu; Mao, Liang; Cai, Xiaoyan; Geng, Zikang; Zhang, Haoyu; Zhang, Junying; Tan, Xin; Ye, Jinhua; Yu, Tao

doi:10.1002/adfm.202213901

Cited by 41 publications

(15 citation statements)

References 45 publications

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“…The actual Cu content of HCC@Cu is confirmed by the ICP-MS results (Table S1), which is consistent with Cu/HCC-2. Of particular interest here is that no signal of Cu 2p is detected for Cu/HCC-2, while two peaks at 932.4 eV (Cu 2+ 2p 3/2 ) and 952.2 eV (Cu 2+ 2p 1/2 ) are observed for HCC@Cu. Although HCC@Cu and Cu/HCC-2 have the same Cu weight percentage, the high-resolution XPS spectra of the Cu 2p signal of the two samples are significantly different.…”

Section: Results and Discussionmentioning

confidence: 91%

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO₂ Reduction

Ma,

Zhang,

Xie

et al. 2024

ACS Catal.

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Doping engineering has enabled the construction of homogeneous and abundant atomic-level catalytic sites for photocatalytic CO 2 reduction with improved selectivity for the target product. However, little is known about the effect of the spatial position of the heteroatoms on the photocatalytic activity of the semiconductors toward CO 2 reduction. Herein, uniform Cu doping into the bulk phase of hollow CdS cubes (HCC) and Cu doping onto the surface of HCC, denoted as Cu/HCC and HCC@ Cu, respectively, are prepared by tuning the introduction order of Cu sources. Experimental analysis shows that the introduction of Cu by both methods can promote the separation and migration of photoinduced charge carriers in CdS. Notably, Cu doping onto the surface of CdS in HCC@Cu leads to much better proton reduction to H 2 production performance but lower CO 2 reduction efficiency as compared to bare CdS. In sharp contrast, Cu doping into the bulk phase of CdS enhances the CO 2 -to-CO conversion while mitigating H 2 evolution. This should be ascribed to the smaller overpotential of Cu/HCC in the CO 2 saturated system than that in the Ar system. In addition, doping Cu atoms into the bulk phase of CdS shifts the d band center of Cu/HCC upward to near the Fermi energy level, which promotes the adsorption and activation of CO 2 on CdS. These results indicate that the photoelectrons with a prolonged lifetime in Cu/HCC preferably reduce CO 2 molecules rather than protons. The density functional theory (DFT) calculation results show that the introduction of Cu heteroatoms can promote the desorption of CO*, and the adaptable sulfur vacancies (Vs) produced by in situ doping techniques can stimulate the formation of CO* intermediates, resulting in the high performance of photocatalytic CO 2 reduction to CO. This work reveals the effect of different heteroatom doping locations on the catalytic activity and will provide a reference for the design of efficient photocatalysts with atomic-level fine structure.

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Section: Results and Discussionmentioning

confidence: 91%

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO₂ Reduction

Ma,

Zhang,

Xie

et al. 2024

ACS Catal.

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“…The intermediates of the new pathway could be adsorbed on the surface Ti and oxygen vacancies, greatly reducing the reaction energy barrier. Wang et al 133 prepared ultrathin CuGaS 2 / Ga 2 S 3 nanosheets with S vacancies with a thickness of only 1.3 nm by a simple hydrothermal method, as shown in Figure 12(a). The ultrathin nanosheets facilitated the charge separation.…”

Section: Co 2 Reductionmentioning

confidence: 99%

“…(a) AFM image of ultrathin CGS/GS. (b) Time-dependent conversion yield of CO 2 into C 2 H 4 with different samples . (a, b) Reproduced with permission from ref .…”

Section: Application Of Surface Engineering In Photocatalysismentioning

confidence: 99%

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Progress and Outlook of Surface Engineering Strategies in Photocatalytic Materials for Mercury Removal: A Review

Yang,

Wu,

et al. 2023

Energy Fuels

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In recent years, the potential of photocatalysis for environmental purification and energy conversion has been gradually explored. However, the limited light absorption and easy recombination ability of photogenerated carriers limit its development. To promote the photocatalytic reaction, the surface modification of photocatalytic materials is usually performed to enhance the photocatalytic activity. This review first presents the recent research progress of surface engineering strategies in photocatalytic oxidation of elemental mercury. Then the mechanism of surface engineering strategies to promote photocatalytic oxidation of Hg0 reaction is analyzed at the level of energy band structure, carrier separation, and molecular activation. Next, the application of surface engineering strategies in photocatalysis is described, including environmental purification and energy conversion. Finally, future opportunities and challenges for the development of photocatalysis are presented. This review can not only provide scientific and theoretical guidance for the modification design of photocatalytic materials but also provide strong support for the preparation of photocatalysts for energy conversion and environmental remediation.

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“…A series of intricate chemical processes is indispensable to convert CO 2 and realize turning "waste" into a treasure. At present, CO 2 reduction reaction (CO 2 RR) products can be divided into CO, [5][6][7][8] CH 4 , [9][10][11] CH 3 OH, [12][13][14] HCOOH, [15][16][17] C 2 H 4 , [18][19][20][21] C 2 H 5 OH 22 , and some other chemical compounds 23,24 according to the types of catalysts. Among them, C 2 H 4 has garnered significant attention from researchers for its versatility and usefulness as a raw material in the synthesis of many chemicals.…”

Section: Introductionmentioning

confidence: 99%

Tandem catalysts CuSe/Au_X for increasing local *CO concentration to promote the photocatalytic CO₂ reduction to C₂H₄

Yan,

Wang,

et al. 2023

Electron

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It is highly desired yet challenging to strategically steer CO2 reduction reaction (CO2RR) toward ethylene (C2H4) with high activity under visible light irradiation. The key to achieving this goal is increasing the local *CO concentration on the catalyst surface and promoting the C‐C coupling progress. Here, we prepare tandem catalysts of CuSe/AuX to realize the photocatalytic reduction of CO2 to C2H4 with high activity. Under light irradiation, the loaded Au NPs are used to activate and transfer CO2 to *CO. The generated *CO intermediate could migrate to the surface of CuSe and cause the C‐C coupling process. Moreover, the theoretical calculation results show that the transport process of *CO from Au NPs to CuSe is spontaneous, which plays a critical role in guaranteeing the high concentration of *CO intermediate on the surface of CuSe. This work not only reveals the effect of tandem catalysis on CO2RR to C2 products but also explores the most suitable tandem catalyst to produce C2H4 with high activity by adjusting the loading amounts of Au NPs. Thus, it provides a way to adjust the Cu‐based catalyst used in the production of C2 products by photocatalytic CO2RR, which may attract extensive attention in the field.

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Regulating the Metallic Cu–Ga Bond by S Vacancy for Improved Photocatalytic CO₂ Reduction to C₂H₄

Cited by 41 publications

References 45 publications

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO₂ Reduction

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO₂ Reduction

Progress and Outlook of Surface Engineering Strategies in Photocatalytic Materials for Mercury Removal: A Review

Tandem catalysts CuSe/Au_X for increasing local *CO concentration to promote the photocatalytic CO₂ reduction to C₂H₄

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Regulating the Metallic Cu–Ga Bond by S Vacancy for Improved Photocatalytic CO2 Reduction to C2H4

Cited by 41 publications

References 45 publications

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO2 Reduction

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO2 Reduction

Progress and Outlook of Surface Engineering Strategies in Photocatalytic Materials for Mercury Removal: A Review

Tandem catalysts CuSe/AuX for increasing local *CO concentration to promote the photocatalytic CO2 reduction to C2H4

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Product

Resources

About

Regulating the Metallic Cu–Ga Bond by S Vacancy for Improved Photocatalytic CO₂ Reduction to C₂H₄

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO₂ Reduction

Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO₂ Reduction

Tandem catalysts CuSe/Au_X for increasing local *CO concentration to promote the photocatalytic CO₂ reduction to C₂H₄