ELECTROCHIMICA ACTA
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2025
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IF 5.6
Xu Ji,Weicong Xu,Chao Liu,Xing Wang
The electrocatalytic CO₂ reduction reaction (CO₂RR) offers a promising pathway for carbon cycling and high-value fuel synthesis. However, the efficient production of ethylene (C₂H₄), a critical multicarbon product, remains constrained by insufficient catalyst activity and selectivity. Although copper-based materials enable C–C coupling, conventional CuO catalysts suffer from imbalanced *CO intermediate adsorption strength and sluggish charge transfer kinetics.In this study, a silica (SiO₂) doping strategy was employed to synergistically modulate the electronic structure and surface active site distribution of CuO, significantly enhancing CO₂-to-C₂H₄ conversion efficiency. Experimental results demonstrate that SiO₂ incorporation induces local electronic density rearrangement around Cu²⁺, stabilizing *CO adsorption, while the constructed Cu-O-Si interfaces accelerate charge transfer, enhances electron transfer and reduce the energy barrier for *COCHO formation. The optimized SiO₂-10%/CuO catalyst achieves a C₂H₄ Faraday efficiency of 42% and a partial current density of 6.3 mA/cm² at −1.4 V (vs. RHE), representing a threefold improvement over pristine CuO. Notably, the catalyst exhibits exceptional stability over 4 hours.Structural characterization and theoretical calculations reveal that SiO₂ doping promotes the self-assembly of CuO nanosheets into flower-like architectures with a high specific surface area and exposes synergistic (111)/(002) facets, which collectively enhance *CO intermediate enrichment and directional coupling. This work provides novel insights into designing high-performance CO₂RR catalysts through multidimensional modulation strategies.
研究领域:
材料科学
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电化学
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DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 6
·2435
·
IF 4.6
Fulin Wang,Zhenzhen Yu,Kaiyang Shi,Xiangwei Li,Kangqiang Lu,Weiya Huang,Changlin Yu,Kai Yang
The green and clean sunlight-driven catalytic conversion of CO2into high-value-added chemicals can simultaneously solve the greenhouse effect and energy problems. The controllable preparation of semiconductor catalyst materials and the study of refined structures are of great significance for the in-depth understanding of solar-energy-conversion technology. In this study, we prepared nitrogen-doped NiO semiconductors using a one-pot molten-salt method. The research shows that the molten-salt system made NiO change from p-type to n-type. In addition, nitrogen doping enhanced the adsorption of CO2on NiO and increased the separation of photogenerated carriers on the NiO. It synergistically optimized the CO2-reduction system and achieved highly active and selective CO2photoreduction. The CO yield on the optimal nitrogen-doped photocatalyst was 235 μmol·g−1·h−1(selectivity 98%), which was 16.8 times that of the p-type NiO and 2.4 times that of the n-type NiO. This can be attributed to the fact that the nitrogen doping enhanced the oxygen vacancies of the NiOs and their ability to adsorb and activate CO2molecules. Photoelectrochemical characterization also confirmed that the nitrogen-doped NiO had excellent electron -transfer and separation properties. This study provides a reference for improving NiO-based semiconductors for photocatalytic CO2reduction.Keywords:NiO;nitrogen doping;photocatalysis;reduction of CO2
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Jiajing Zhang,Suwei Wang,Pin Song,Ang Li,Wei Jiang,Jun Di
The insufficient solar light response ability of the photocatalyst, rapid recombination of interface charges, and lack of active sites significantly inhibit the efficiency of photocatalytic CO 2 reduction. Addressing these challenges simultaneously is a very challenging task. Herein, an interface engineering coupled surface polarization strategy is proposed to optimize the CO 2 photoreduction performance. The copper tetracarboxyphenylporphyrin (CuTCPP) modified BiOBr/Bi 19 S 27 Br 3 (BBS) heterostructure was developed. The built-in electric field formed between BiOBr and Bi 19 S 27 Br 3 interfaces induces the effective interfacial charge separation, while the surface polarization of CuTCPP induces the transfer of electrons from the conduction band (CB) of BBS to the CB of CuTCPP. Benefiting from this unique configuration and abundant active sites in CuTCPP, greatly improved photocatalytic CO 2 reduction performance can be realized. Without adding cocatalysts and sacrificial agents, the optimized CO generation performance of CuTCPP-BiOBr/Bi 19 S 27 Br 3 (BBS-CT) is 3.5 times higher than that of BBS. This work provides valuable insights of interface engineering coupled surface polarization strategy for collaborative improve the photocatalytic CO 2 reduction performance.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xin Li,Jingru Guan,Haopeng Jiang,Xianghai Song,Pengwei Huo,Huiqin Wang
Construction of multi-interface contact step-scheme (S-scheme) photocatalyst is a promising pathway to achieve high-electron transfer efficiency for photocatalytic CO 2 reduction. In this paper, g-C 3 N 4 nanosheets were selected as the main photocatalyst, rod-like CeO 2 (R-CeO 2 ) with unique Ce 4+ →Ce 3+ conversion property and rGO were loaded on the g-C 3 N 4 surface to construct 2D-1D-2D sandwich photocatalyst. The yields of CO and CH 4 were about 63.18 and 32.67 μmol/g after 4 h when the rGO/R-CeO 2 /g-C 3 N 4 was used as catalyst, which were about 4 and 6 times higher than that of pure CN, respectively. Cyclic experiments proved that the composite had excellent photocatalytic and material stability. Photoelectrochemical tests showed that the construction of S-scheme electron transfer model and the introduction of rGO can great enhance the electron transmission and separation of photogenerated electron-hole pairs. CO 2 adsorption test identified that the loading of R-CeO 2 and rGO obviously enhanced the CO 2 adsorption ability of pure g-C 3 N 4 . Density functional theory (DFT) calculations used to analyze the electron transfer path and the formation of the build-in electric field at the semiconductor interface. In-situ FTIR and 13 CO 2 element-tracer detection carried out to research the process of CO 2 photoreduction. A possible multi-interface contact S-scheme electron transfer mechanism for enhanced CO 2 photoreduction activity has been discussed.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 15
·4525-4533
·
IF 5
Qiuyu Zhang,Yajie Chen,Xinyan Yu,Yuejia Yin,Yaxin Ru,Guohui Tian
Fabricating photocatalysts with customizable structure and composition using different metal–organic framework (MOF) building blocks has intriguing implications in chemistry and material science, but it is challenging to do so. Here, a two-step synthetic strategy was designed to prepare MIL-125(Ti)@TiO2 hollow nanodiscs decorated with Co3S4 nanoparticles for CO2 photoreduction. The Co-based zeolite imidazolium ester backbone (ZIF-67) nanolayer was first loaded on the prepared MIL-125(Ti) nanodiscs to form core@shell MIL-125(Ti)@ZIF-67 nanodiscs. The following sulfidation process under solvothermal condition led to the production of MIL-125(Ti)@TiO2 hollow nanodiscs decorated with Co3S4 nanoparticles (MIL-125(Ti)@TiO2\Co3S4). This ternary hybrid catalyst with hollow nanodisc structure possessed a significantly enhanced charge separation efficiency and visible light absorption, along with offering a huge number of active sites. Considering the above advantages, the CO2 photoreduction activity of the optimized MIL-125(Ti)@TiO2\Co3S4 catalyst was significantly increased when compared to single-component catalysts (MIL-125(Ti), TiO2, and Co3S4) and binary hybrid catalysts (MIL-125(Ti)@TiO2 and TiO2\Co3S4) under simulated sunlight irradiation. CO is the main product with a productivity of 587.50 μmol g−1 h−1, which is almost seven times higher than that of pure MIL-125(Ti). The potential photocatalytic mechanism of the hybrid photocatalyst has also been demonstrated. This study presents a simple and effective technique for fabricating MOF-based hybrid catalysts for photocatalytic applications.
研究领域:
材料科学
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化学
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DOI
高影响因子
INORGANIC CHEMISTRY
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2022
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IF 5.436
Yimeng Zhou,Qianjin Ye,Xiangli Shi,Qiong Zhang,Qi Song,Changjian Zhou,Di Li,Deli Jiang
Due to the multiple electron and proton transfer processes involved, the photogenerated charges are easily recombined during the photocatalytic reduction of CO2, making the generation of the eight-electron product CH4 kinetically more difficult. Herein, Ni3B nanoparticles modulated by p-block element were combined with TiO2 nanosheets to construct a novel Schottky junction photocatalyst (Ni3B/TiO2) for the selective photocatalytic conversion of CO2 to CH4. The formed Ni3B/TiO2 photocatalyst with Schottky junction ensures a transfer pathway of photogenerated electrons from TiO2 to Ni3B, which facilitates the accumulation of electrons on the surface of Ni3B and subsequently improves the activity of photocatalytic CO2 reduction to CH4. The optimized Ni3B/TiO2 Schottky junction shows an improved CH4 yield of 30.03 μmol g–1 h–1, which was much higher than those of TiO2 (1.62 μmol g–1 h–1), NiO/TiO2 (2.44 μmol g–1 h–1), and Ni/TiO2 (4.3 μmol g–1 h–1). This work demonstrated that the introduction of p-block elements can alleviate the scaling relationship effect of pure metal cocatalysts to a certain extent, and the modified Ni3B can be used as a promising new cocatalyst to effectively improve the selective photocatalytic of CO2 to CH4.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Shangguan Wenchao,Liu Qing,Wang Ying,Sun Ning,Liu Yu,Zhao Rui,Li Yingxuan,Wang Chuanyi,Zhao Jincai
Achieving CO 2 reduction with H 2 O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO 2 to CO with the help of H 2 O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g −1 h −1 (~100% selectivity), ~2.5 times the rate during CO 2 reduction with H 2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H 2 O decomposition, which synchronously optimizes the rate-determining steps in the CO 2 reduction and H 2 O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O 2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO 2 reduction with H 2 O.
研究领域:
化学
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材料科学
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环境科学
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催化
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Xuandong Wang,Jie He,Liang Mao,Xiaoyan Cai,Chuanzhi Sun,Mingshan Zhu
Photocatalytic CO 2 conversion to valuable fossil fuels has been demonstrated to be a promising approach to reduce emissions of CO 2 and produce renewable energy, which primarily depends on developing the high efficiency of charge separation photocatalysts. Herein, CsPbBr 3 , one typical kind of all-inorganic perovskite nanocrystal, is immobilized on monolayer MoS 2 nanosheets to construct a new and ideal CsPbBr 3 /MoS 2 photocatalyst in the application of CO 2 photoreduction. In comparison with pure CsPbBr 3 , CsPbBr 3 /MoS 2 heterostructures possessed a specific electric field to more efficiently separate charges and generated more active sites for facilitating CO 2 activation, resulting in 3.0 and 2.4 times yields for CO 2 photoreduction to CH 4 and CO, respectively. Detailed characterization methods such as photoluminescence, surface photovoltage spectroscopy and theory calculations indicate the vivid illustrations of photogenerated carries separation which contributes to improving photocatalytic CO 2 conversion efficiency. The present investigation is anticipated to provide a new way for fabricating highly efficient perovskite-based photocatalyst in solar-energy-driven applications.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiangli Shi,Pengfei An,Qiong Zhang,Qi Song,Deli Jiang,Dan Tian,Di Li
Photocatalytic CO 2 conversion into value-added chemicals is a promising strategy to remedy the energy crisis and environmental pollution, yet developing cost-effective photocatalysts that can efficiently and selectively convert CO 2 to desirable products is still a great challenge. Herein, we construct a Fe 2 P nanoparticles decorated on the surface of the nitrogen vacancies (NVs) modified g-C 3 N 4 nanosheet hybrid photocatalyst (Fe 2 P/NVsCN) for photocatalytic conversion of CO 2 to CO. The NVs can significantly improve the visible light absorption due to the formation of midgap state, and the metallic Fe 2 P as the cocatalyst is beneficial to promote the photo-generated charge separation and migration, impede the side reaction, in which improve the activity and selectivity. By adjusting the contents of Fe 2 P and NVsCN, the optimal 20%-Fe 2 P/NVsCN(1:5) sample shows an excellent CO evolution rate in visible light of 22.48 µmol g -1 h −1 with 97.5% selectivity, which is superior to most reported g-C 3 N 4 -based photocatalysts. Furthermore, this photocatalyst also exhibits good stability due to the timely consumption of electrons, and it maintains stable CO evolution rate over 20 h. This work opens a new horizon for design and construction of active photocatalyst with high selectivity by synergistic modulating the surface vacancy and cocatalyst.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Ruijie Chen,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction can simultaneously alleviate the energy crisis and solve environmental issues. Nevertheless, it is still challenging for designing photocatalysts with efficient carrier mobility in rational. Herein, the Bi 2 MoO 6 /g-C 3 N 4 (BMO/CN) heterostructure was constructed through a microwave-assisted which could enhance the construction of two-dimensional and two-dimensional (2D/2D) structures. The 2D/2D BMO/CN heterojunction possessed excellent charge separation efficiency which exhibited superior performance on photocatalytic CO 2 reduction. It was shown by the characterization that the (131) surface of Bi 2 MoO 6 was constructed with the (100) surface of g-C 3 N 4 . The work functions of Bi 2 MoO 6 and g-C 3 N 4 were determined to be 4.57 and 4.22 eV, respectively, which suggested the type-II heterojunction was formed. The formation of CO and CH 3 OH over the optimized BMO/CN-30% catalyst reached 2.44 and 3.61 µmol⋅g −1 ⋅h −1 , respectively. The immediate products of HCO 3 - were observed within in-situ FT-IR to further certify the evolution of CH 3 OH. This work highlighted a microwave-assisted strategy to build a heterojunction structure for enhancing photoreduction CO 2 .
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 35
·19681-19686
·
IF 12.732
Zhongjie Yang,Caoyu Yang,Jianyu Han,Wenshi Zhao,Shengxian Shao,Siyu Li,Huiwen Gao,Haijiao Xie,Xiaofei Zhang
Selective electrochemical CO2 reduction to formic acid is an appealing strategy to achieve efficient utilization of CO2. Modification of the catalytic interface with organic linkers has been proven to promote the conversion of CO2 to CO, but the highly selective generation of formic acid is still a challenge. Herein, modification of the interface of graphene oxide (GO) with amide linkages to anchor SnO2 nanoparticles is presented to catalyze the CO2 reduction reaction (CO2RR). As expected, the as-synthesized SnO2/tert-GO shows a competitive high cathodic faradaic efficiency (FE) of 84.4% for formate at −0.96 V and shows long-term stability for the CO2RR. Further, density functional theory (DFT) calculations indicated that amide linkages facilitate the conversion of CO2 to formate.
研究领域:
电化学
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材料科学
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催化
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Jia Li,Wentao Liu,Yang Li,Zhi Liu,Yang Liu
A series of hierarchical flower-like CdS/carbon quantum dots/NiAl-LDH (CCL) photocatalyst have been successfully prepared to achieve efficient conversion of CO 2 -to-CO via a simple yet effective hydrothermal method. In the CCL, interspersed-CQDs not only increase the number of reactive sites but also reduce inner electronic impedance with the assistance of light reflecting-scattering effect. This significantly improves electron migration efficiency and inhibits the recombination of photoinduced electron-holes pairs. Without any sacrificial agent or photosensitizer, the sample of CCL-1 exhibits the highest CO evolution rate of 7.04 μmol·g −1 ·h −1 in water under simulated sunlight illumination with a large specific surface area (129.15 m 2 g −1 ) and an appropriate CQDs content of 15.2 wt%, which is 12.8- and 11.2-fold higher than those of pristine LDH, pure CdS, and many previously reported LDH-based counterparts. A type-Ⅱ interfacial charge transfer mechanism is proposed, where electrons migrate rapidly from CdS to LDH with highly-interspersed CQDs as unhindered electron conduction bridges. The present work outlines a simple and controllable LDH-based heterojunction, which give rise to superior photocatalytic activity for CO 2 photoreduction.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
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