INORGANIC CHEMISTRY
·
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
Surfaces and Interfaces
·
2025
·
IF 6.3
Chaoqiang Li,Xiangyu Xu,Aizhong Jia
Photocatalytic reduction of CO 2 to chemical fuels is a promising strategy to alleviate the greenhouse effect and energy crisis. This article successfully fabricated Ag/CdS composites with ohmic junction using a two-step method and further verified them by DFT calculations. Meanwhile, photoelectrochemical and electron paramagnetic resonance tests show that Ag/CdS has higher photocurrent density and lower charge transfer resistance, suggesting that the ohmic junction achieves ultrafast electron transfer from CdS to Ag under light irradiation, significantly promoting the separation of photogenerated carriers. Furthermore, the localized plasmon resonance (LSPR) of Ag enhances the light absorption of the catalyst and generates a large number of hot electrons for the photocatalytic reduction reaction. The synergistic effect of ohmic junction and LSPR gives high electron density at the reaction site, which promotes the multiple proton-coupled electron reactions leading to highly selective photoconversion of CO 2 to CH 4 . Under the optimized conditions, the CH 4 yield of the synthesized Ag/CdS is 68.6 μmol·g −1 ·h −1 , which is 25.4 times higher than that of bare CdS, and the CH 4 selectivity increases from 53.8% to 90.1%. This study provides a new idea for the design of CdS-based materials for highly selective reduction of CO 2 to CH 4 .
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
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Deli Jiang,Yimeng Zhou,Qianxiao Zhang,Qi Song,Changjian Zhou,Xiangli Shi,Di Li
Photocatalytic reduction of CO2 toward eight-electron CH4 product with simultaneously high conversion efficiency and selectivity remains great challenging owing to the sluggish charge separation and transfer kinetics and lack of active sites for the adsorption and activation of reactants. Herein, a defective TiO2 nanosheet photocatalyst simultaneously equipped with AuCu alloy co-catalyst and oxygen vacancies (AuCu-TiO2–x NSs) was rationally designed and fabricated for the selective conversion of CO2 into CH4. The experimental results demonstrated that the AuCu alloy co-catalyst not only effectively promotes the separation of photogenerated electron–hole pairs but also acts as synergistic active sites for the reduction of CO2. The oxygen vacancies in TiO2 contribute to the separation of charge carriers and, more importantly, promote the oxidation of H2O, thus providing rich protons to promote the deep reduction of CO2 to CH4. Consequently, the optimal AuCu-TiO2–x nanosheets (NSs) photocatalyst achieves a CO2 reduction selectivity toward CH4 up to 90.55%, significantly higher than those of TiO2–x NSs (31.82%), Au-TiO2–x NSs (38.74%), and Cu-TiO2–x NSs (66.11%). Furthermore, the CH4 evolution rate over the AuCu-TiO2–x NSs reaches 22.47 μmol·g–1·h–1, which is nearly twice that of AuCu-TiO2 NSs (12.10 μmol·g–1·h–1). This research presents a unique insight into the design and synthesis of photocatalyst with oxygen vacancies and alloy metals as the co-catalyst for the highly selective deep reduction of CO2.
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
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2018
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IF 8.097
Dongxing Tan,Jianling Zhang,Jinbiao Shi,Shaopeng Li,Bingxing Zhang,Xiuniang Tan,Fanyu Zhang,Lifei Liu,Dan Shao,Buxing Han
To develop photocatalysts with desirable compositions and structures for improving the efficiency and selectivity of CO2 conversion to CH4 under mild conditions is of great importance. Here, we design an effective photocatalyst of bimetal (Ag/Pd) nanoalloys supported on nitrogen-doped TiO2 nanosheet for CO2 conversion. Such a novel photocatalyst combines multiple advantages of abundant Ti3+ ions, oxygen vacancies, and substitutional nitrogen that are favorable for catalyzing CO2 reduction. It was found that CO2 could be efficiently transformed to CH4 under mild conditions, i.e., in aqueous solution and at atmospheric pressure and room temperature. The maximum production rate of CH4 can reach 79.0 μmol g–1 h–1. Moreover, the Ag/Pd bimetals supported on N-doped TiO2 nanosheet exhibit high selectivity to CH4. The as-synthesized photocatalyst can be well recycled for CO2 reduction.
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
Green Energy & Environment
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2025
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IF 14.6
Jinshan Chen,Jiangfeng Lu,Ran Lang,Chi Wang,Shuangyou Bao,Yuan Li,Kai Li,Maohong Fan
In this study, a novel Pt-loaded CuPc/g-C 3 N 4 (PtCuCN) composite was synthesized for the selective photocatalytic reduction of CO 2 to CH 4 under visible light. The PtCuCN catalyst achieved a CH 4 yield of 39.8 μmol g⁻ 1 h⁻ 1 , significantly outperforming bulk g-C₃N₄ and CuPc alone by factors of 2.5 and 3.1, respectively, with a high selectivity of 90%. In comparison with other commonly studied photocatalysts, such as g-C 3 N 4 -based catalysts, the PtCuCN composite exhibited superior CH 4 yield and product selectivity, demonstrating its potential as a more efficient photocatalyst for CO₂ reduction. X-ray photoelectron spectroscopy (XPS), density functional theory (DFT) calculations, and in-situ infrared (IR) analysis revealed that the Pt⁰ species effectively lower the activation energy for CH 4 formation, while CuPc extends the light absorption range and enhances charge separation. The combined effects of these components in a Z-scheme heterojunction provide new insights into designing highly selective CO 2 -to-CH 4 photocatalysts. This work demonstrates the potential of PtCuCN as a highly efficient and stable catalyst for CO 2 reduction to CH 4 under visible light.
研究领域:
材料科学
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环境科学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2019
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IF 7.723
Jiaxuan Fan,Lingxiang Cheng,Yanan Liu,Yufei He,Yanfei Wang,Dianqing Li,Junting Feng
Photocatalytic reduction of CO 2 with H 2 O into CH 4 is a promising way to realize solar energy utilization and CO 2 conversion, in which the key issue is how to enhance and couple CO 2 reduction as well as H 2 O oxidation. In this work, we precisely fabricated a binary functional photocatalyst by loading Au@Pd nanoparticles onto V O -rich TiO 2 through a surfactant-free deposition-reduction method, whose fine structure was confirmed by aberration-corrected HAADF-STEM, EELS, EPR and XPS. Combining photocatalytic performance with a series of in situ FTIR measurements, we clarified the role of metallic sites and semiconductor support in coupling CO 2 reduction and H 2 O oxidation. Specifically, H 2 O oxidation process was facilitated by the V O -rich TiO 2 to contribute more protons, followed by the activation of CO 2 and protons primarily by the metallic Au@Pd sites to form the surface bounded Au@Pd-CO 2 − and Au@Pd-H species. By adjusting the ratio of Au@Pd nanoparticles and V O concentration to manipulate the Au@Pd-CO 2 − /Au@Pd-H ratio, CH 4 yield of 26.32 μmol/(g·h) and selectivity of electron toward CH 4 of 96% can be observed with minimal concomitant H 2 generation. These findings could open a feasible and universal route to enhance the photocatalytic efficiency of CO 2 conversion.
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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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Hongli Yang,Huilin Hou,Man Yang,Zhongli Zhu,Hui Fu,Dongdong Zhang,Yong Luo,Weiyou Yang
The selective photoreduction of CO 2 into hydrocarbon fuels, such as CH 4 , is highly desirable for sustainable energy but remains a significant challenge due to slow proton-electron transfer processes and competing intermediates. Herein, a novel NiO/MgAl-LDH (NMA-x, LDH represents layered double hydroxide) step-scheme (S-scheme) heterojunction has been engineered via in-situ anchoring MgAl-LDH nanoplates on metal–organic frameworks (MOFs) derived NiO microrods, which improves the CO 2 adsorption capability and specific surface area of NiO. The steered internal electric field in the p-n heterointerface promotes charge separation and attracts a high electron density center on the catalyst surface to favor CH 4 production. Meanwhile, S-scheme photogenerated charge transfer mechanism is proposed by in-situ X-ray photoelectron spectroscopy (XPS), in-situ diffuse reflectance infrared Fourier transform (DRIFT) spectra and density functional theory (DFT) calculation. In this process, photogenerated electrons are transferred from the conduction band (CB) of MgAl-LDH to the valence band (VB) of NiO, facilitating the CHO* species serve as the critical intermediate for producing CH 4 through desired photocatalytic CO 2 reduction. Using pure water as a proton source, the NMA-2 catalyst achieved a high CH 4 selectivity of 91.2% and a yield of 8.98 μmol∙g −1 ∙h −1 , representing significant potential for practical applications. This catalyst outperformed pristine and revitalized NiO by 4.23 and 2.07 times, respectively.
研究领域:
材料科学
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催化
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环境化学
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光化学
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产品关联
DOI
高影响因子
ADVANCED ENGINEERING MATERIALS
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2023
·Vol. 25
·期 22
·2301062
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IF 3.6
Binxia Yuan,Hong Qian,Lan Cao,Rui Zhu,Weiling Luan
Herein, H + in oxalic acid is used instead of Na + to obtain titanate nanosheets through P200 hydrolysis, which further curls to form a multilayer TiO 2 nanotubes (NTs) structure. Then, Cu 2 O quantum dots (QDs) are successfully loaded on TiO 2 NTs via a hydrothermal method using fructose as a reducing agent. The optical, impedance, and photocurrent tests indicate that the composite structure improves its optoelectronic performance. The photocatalytic H 2 production and CO 2 reduction efficiency of Cu 2 O QDs/TiO 2 NTs are lower than those of TiO 2 NTs. However, the molar ratio of CH 4 to CO produced by CO 2 reduction of Cu 2 O QDs/TiO 2 NTs composite catalyst is greater than that of pure TiO 2 NTs. The CH 4 production accounts for 97%, indicating that the composite catalyst has a high CH 4 selectivity. The experimental and density functional theory calculation results prove that the Z-scheme heterojunction accelerates the separation and transfer of photogenerated carriers, and broadens the absorption range of visible light.
研究领域:
材料科学
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纳米技术
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环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Ya-Nan Jing,Xing-Liang Yin,Lei-Lei Li,Yan-Lan Wang,Jia Xue,Ze-Feng Xu,Da-Qiang Liu,Chuan-Wu Chen,Xiao-Jie Liu,Er-Kang Liu
CO 2 -to-high value-added chemicals via a photocatalytic route is of interest but strangled by the low efficiency. Herein, a novel Fe-TiO 2-x /TiO 2 S-scheme homojunction was designed and constructed by using a facile surface modification approach whereby oxygen vacancy (OV) and Fe introducing on the TiO 2 nanorod surface. The as-synthesized Fe-TiO 2-x /TiO 2 S-scheme homojunction exhibits positive properties on promoting photocatalytic CO 2 reduction: i) the nanorod structure provides numerous active sites and a radical charge transfer path; ii) the doped Fe and OV not only synergistically enhance light utilization but also promote CO 2 adsorption; iii) the Fe-TiO 2-x /TiO 2 S-scheme homojunction benefits photoexcited charge separation and retains stronger redox capacity. Thanks to those good characters, the Fe-TiO 2-x /TiO 2 homojunction exhibits superior CO 2 reduction performances with optimized CO/CH 4 generation rates of 122/22 μmol g -1 h −1 which exceed those of pure TiO 2 by more than 9.4/7.3 folds and most currently reported catalytic systems. This manuscript develops a facile and universal approach to synthesize well-defined homojunction and may inspire the construction of other more high-efficiency photocatalysts toward CO 2 reduction and beyond.
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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催化
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DOI
PubMed
高影响因子
RARE METALS
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2024
·
IF 9.6
Wan Si-Jie,Hou Yan-Ting,Wang Wang,Luo Guo-Qiang,Wang Chuan-Bin,Tu Rong,Cao Shao-Wen
Photocatalytic reduction of CO 2 has attracted considerable interest owing to its potential to resolve the energy and environmental problems. Nevertheless, the lack of proficient photocatalysts has restricted the application of solar-driven photocatalytic CO 2 reduction. Herein, we reported an S-scheme heterojunction by combining g-C 3 N 4 with La 3+ and Rh 3+ co-doped SrTiO 3 through the electrostatic self-assembly method for the efficient photocatalytic CO 2 reduction. In comparison with g-C 3 N 4 , the as-prepared CN/LRSTO-30 wt% S-scheme heterojunction not only possesses a broadened visible-light response due to the defect states in La, Rh co-doped SrTiO 3 induced by co-doped La 3+ and Rh 3+ but also has more adsorption sites for the capture and activation of CO 2 molecules. Additionally, separation and transfer efficiency of the photoinduced charge carriers is much enhanced in the CN/LRSTO-30 wt% S-scheme heterojunction via its robust internal electric field, which is firmly demonstrated by in situ irradiation X-ray photoelectron spectroscopy technology. Consequently, the prepared S-scheme heterojunction achieves impressive photocatalytic CO 2 reduction performance with an average CO and CH 4 evolution rate of 4.1–1.8 μmol·g −1 ·h −1 , respectively, which are ~ 1.9 and ~ 22.5-fold higher than those of pure g-C 3 N 4 . This study provides innovative perspectives on the design of creative S-scheme heterojunctions for applications in photocatalytic CO 2 reduction. Graphical abstract
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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能源科学
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产品关联
DOI
高影响因子
APPLIED ENERGY
·
2020
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IF 8.848
Hou-Yun Yang,Yi-Xuan Wang,Chuan-Shu He,Yuan Qin,Wen-Qiang Li,Wei-Hua Li,Yang Mu
Regulating cathodic interface properties towards highly effective CH 4 production from CO 2 is of great importance for energy storage using microbial electro-synthesis (MES). Herein, the feasibility and mechanism of two typical redox mediators , neutral red (NR) and anthraquinone-2, 6-disulfonate (AQDS), were evaluated for the improvement of CH 4 formation from CO 2 reduction in mixed-culture biocathodes of MESs. Results showed that the CH 4 formation rates of biocathodes after modification with NR and AQDS were 5.8 and 3.5 times higher than that of unaltered cathodes. Moreover, the coulombic efficiency of CH 4 formation improved from 44.27 ± 4.01% of the control cathode to 64.30 ± 4.83% and 62.26 ± 2.87% after modification with NR and AQDS, respectively. Consequently, the energy efficiency of MESs after cathode modification with NR and AQDS increased to 58.33 ± 3.17% and 53.21 ± 4.11% compared to 38.20 ± 3.12% without modification. Such improvements were likely attributed to the enhanced extracellular electron transfer of microbes, the reduction in internal resistances and the enrichment of hydrogenotrophic methanogens in the mixed-culture biocathodes after modification with NR and AQDS. This study provides an alternative strategy to regulate cathodic interface in MESs for renewable energy storage and biomethane production from CO 2 .
研究领域:
环境科学
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生物技术
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电化学
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微生物学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）