APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Baiyan Zhang,Chaoqiu Chen,Jian Liu,Wei Qiao,Jixiao Zhao,Jie Yang,Yu Yu,Shuai Chen,Yong Qin
Heteroatom doping and loading of co-catalysts are two efficient tactics to boost the photocatalytic activity of semiconductors. Combining these two strategies in one photocatalyst system has great potential to further enhance the catalytic performance. Herein, a facile and controllable atomic layer deposition (ALD)-reduction approach is used to simultaneously introduce Ni doping and Ni nanoparticles (NPs) with tunable size on CdS nanorods for boosting its photocatalytic activity. The Ni doping and Ni NPs synergistically enhance the H 2 production of CdS nanorods (NRs), achieving an optimized rate of 20.6 mmol·g −1 ·h −1 ~1.3- and 28.6-fold higher than CdS NRs supported Ni NPs with similar size and pristine CdS NRs , respectively. The Ni NPs/Ni doped CdS NRs exhibits an apparent quantum efficiency (AQE) of 37.5% at 420 nm, outperforming most previously reported Ni doped and Ni NPs decorated CdS catalysts. The outstanding photocatalytic activity of the Ni NPs/Ni doped CdS NRs can be ascribed to synergism of the Ni doping and uniformly dispersed Ni co-catalyst with appropriate size, which promote carrier separation of semiconductor and surface hydrogen evolution kinetics on nanocatalyst surface. This work provides a promising pathway to integrate heteroatom doping and loading of co-catalysts strategies in one photocatalyst system for synergistically promoting photocatalytic performance.
研究领域:
材料科学
·
化学工程
·
能源科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xiaoman He,Zhangdi Peng,Peilin Shen,Chenjia Miao,Jiale Xie,Chen Deng,Panagiotis G. Kougias,Dekui Shen,Richen Lin
Conversion of CO2 and H2 into biomethane is a promising technology within the concept of power-to-X. However, the integration of high-value-added products can enhance the economic viability and diversify future biobased production chains. Herein, an integrated biosystem converting CO2/H2 into acetic acid, which is further converted to C4+ fatty acids, was demonstrated with the aim to assess the role of carbonaceous materials (model nanomaterial graphene and cost-effective biochar) and external electron donor (ethanol). With the supplementation of ethanol as the electron donor, carbonaceous materials significantly increased the production and selectivity of butyrate (C4) and caproate (C6) due to enhanced microbial growth and chain elongation efficiency. The highest concentration of butyrate (2512.35 ± 60.05 mg/L) was observed in the graphene-added group, while the highest concentration of caproate (396.74 ± 14.83 mg/L) was observed in the biochar group, suggesting different mechanisms induced by carbonaceous materials. Microbial community analysis revealed that carbonaceous materials primarily enriched members of the genus Clostridium_sensu_stricto_12, which are identified as typical carbon chain elongating microorganisms. Functional prediction revealed that carbonaceous materials increased the relative abundance of functional genes encoding crucial enzymes involved in both the Wood–Ljungdahl pathway and the fatty acid biosynthesis pathway. This study demonstrated an integrated approach for the efficient conversion of CO2 to value-added green chemicals.
研究领域:
环境生物学
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微生物学
·
合成生物学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Peng Liu,Furong Ye,Changcun Han,Chenxi Gao,Huai Yang,Xupeng Chen,Yizhong Huang
Photocatalytic water splitting for green H 2 offers a renewable-energy route, yet efficiency is still limited by poor charge separation and slow reaction kinetics. Here, we report a 2D/2D Ti 3 CN/g-C 3 N 4 heterojunction with a built-in electric field, synthesized via Lewis acid molten-salt etching and electrostatic self-assembly. The heterojunction promotes directional electron transfer from g-C 3 N 4 to Ti 3 CN, while Ru nanoparticles further enhance charge density and reduce the reaction barrier. The optimized Ru/Ti 3 CN/g-C 3 N 4 photocatalyst delivers a H 2 evolution rate of 4254 μmol g −1 ·h −1 under visible light, 200 times higher than pristine g-C₃N₄, with excellent cycling stability. Experimental and theoretical analyses reveal that the synergistic effects of the polarized interface and Ru cocatalyst significantly improve charge separation and H 2 adsorption kinetics. This work offering a practical route to couple MXene co-catalysts with polarization-induced built-in electric fields for markedly accelerating solar-driven H 2 production.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 8.3
Baker Rhimi,Attiq Ur Rehman,Yuanzhi Hu,Sherif A. El-Khodary,Zhehao Liu,Min Zhou,Karim Harrath,Qiang Ma,Long Zhao,Zhifeng Jiang,Weidong Shi
The development of efficient and stable photocatalysts for hydrogen evolution is crucial for solar-to-fuel conversion. Here, we report Cu-porphyrin (CuTCPP)/oxygen-doped g-C 3 N 4 (O–CN) nanohybrids as high-performance sonophotocatalysts, where strong π–π stacking interactions create robust heterojunctions that promote efficient charge separation and transfer. The optimal 2 % CuTCPP/O–CN2 sample exhibited a 3.3-fold enhancement in H 2 evolution compared to O–CN2 under simulated light coupled with ultrasonication. Experimental results combined with density functional theory (DFT) calculations confirmed the suppression of charge recombination and highlighted the synergistic contribution of ultrasonic excitation with light irradiation. Furthermore, oxygen doping was found to not only reinforce the CuTCPP/O–CN interface but also provides robust anchoring sites for Pt cocatalysts, preventing leaching and aggregation while electronically modulating Pt to optimize its d-band center and H 2 adsorption free energy. These findings provide valuable insights into the rational design of stable and high-active hybrid photocatalysts for solar fuel generation.
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Nano Research
·
2024
·Vol. 17
·期 7
·5835-5844
·
IF 9.5
Liu Yu,Shi Yawen,Wang Hua,Zhang Shengbo
Photocatalytic hydrogen generation from hydrogen storage media is an effective and promising approach for the green hydrogen industry as well as for achieving carbon neutrality goals. However, the lower photocatalytic efficiency due to the limited light trapping capacity, low electron transfer rate, and severe aggregation of nanoparticles caused by high surface energy seriously restricts their practical application. Herein, we constructed a series of donor–acceptor (D–A) type covalent organic frameworks to confine ultrafine bimetallic Pt-based nanoclusters for photocatalytic hydrogen generation from ammonia borane (AB) hydrolysis. Under visible light irradiation at 20 °C, PtCo 2 @covalent organic framework (COF) showed the highest photocatalytic activity with a turnover frequency (TOF) of 486 min −1 . Experiments and density functional theory (DFT) calculations reveal that the high catalytic activity is mainly attributed to the strong electronic interactions between D–A type COF and ultrafine PtCo 2 nanoclusters. Specifically, the D–A type COF can significantly enhance the light-trapping ability by fine-tuning the electron-acceptor type in the framework, and accelerate the photogenerated electron transfer from D–A type COF to PtCo 2 nanocluster, which promotes the adsorption and activation of H 2 O and AB molecules and accelerates hydrogen release. Furthermore, PtCo 2 @COF also exhibited ultra-high durability due to the significantly enhanced resistance to nanocluster aggregation caused by the nanopore confinement effect of D–A type COF. We believe that this work will provide a theoretical guide for the rational design of efficient D–A COF-based catalysts for photocatalysis.
研究领域:
材料科学
·
催化化学
·
能源化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·Vol. 40
·期 14
·4777-4785
·
IF 3.313
Jianmin Chen,Zhang-Hui Lu,Yuqing Wang,Xiangshu Chen,Lei Zhang
In this paper, we reported a facile and effective approach for fabrication of SiO 2 –CoFe 2 O 4 supported dispersed Ag nanoparticles (NPs). The as-synthesized nanocomposites (NCs) were characterized by XRD , TEM, EDX, ICP , XPS and N 2 adsorption-desorption, and used as catalyst for H 2 production from hydrolysis of ammonia borane (AB). A poorly active catalyst of Ag NPs was dramatically converted into a highly active catalyst, in the presence of inactive SiO 2 –CoFe 2 O 4 support. Among all the Ag(0)/SiO 2 –CoFe 2 O 4 NCs catalysts tested, the Ag loading of 0.98 wt% exhibited the highest catalytic activity toward hydrolysis of AB with a highly turnover frequency of TOF = 264 min −1 at room temperature, being higher than that of most reported Ag-based catalysts. Especially, these catalysts can be readily separated from the solution for recycle purpose, and can keep the high activity even after seven times of recycle. These results showed that Ag(0)/SiO 2 –CoFe 2 O 4 NCs prepared in this study are a promising catalyst for hydrogen production from aqueous AB and for developing a highly efficient hydrogen storage system for fuel cell applications .
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·Vol. 46
·期 43
·22508-22518
·
IF 5.816
Zhijun Zhang,Kezhen Chen,Jichang Lu,Qin Zou,Yuhui Zhao,Yongming Luo,Dedong He,Rongtao Li
Sn modified CuO–CeO 2 catalysts with different Sn loadings were prepared by a facile, green and solvent-free method. The effect of Sn/Ce ratio over Sn–Cu–Ce-x (x = 0, 1, 2.5, 5, 7.5) samples on CO activity and O 2 selectivity was investigated. The samples were characterized by various techniques using N 2 -adsorption/desorption, XRD , H 2 -TPR, XPS, Raman and in-situ DRIFTS . It was revealed that stronger interaction between acitve sites and support, higher amounts of Sn 2+ and Ce 3+ , associated with increased amount of oxygen vacancies , were observed on the catalyst of Sn–Cu–Ce-5. As a result, the optimized catalyst displayed an excellent catalytic performance even in the presence of CO 2 and H 2 O. In this sense, probing the Sn modified CuO–CeO 2 catalyst can elucidate some useful keys for the development of high CO 2 and H 2 O-resistance catalyst during CO-preferential oxidation in H 2 -rich streams.
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 8.3
Jingyun Mao,Chengjing Lu,Qingrong Qian,Qinghua Chen,Hun Xue,Fangyuan Cheng
Photocatalytic hydrogen evolution represents a pivotal pathway for clean energy conversion. However, the development of high-performance photocatalysts is often constrained by unsustainable synthesis methods and, more fundamentally, by the limited ability to precisely control the interfacial structure for directed charge transport. Herein, we develop a green synthesis strategy to fabricate a polyaromatic carbon layer-encapsulated TiO 2 heterojunction bridged by interfacial Ti-O-C bonds. This is achieved through the controlled calcination of biomass-derived xylose, yielding carbonaceous layers with well-defined sp 2 -hybridized configurations. The optimized Pt-2X-T300 photocatalyst demonstrates a remarkable hydrogen evolution rate of 8570.9 μmol g −1 h −1 under visible light, which is approximately 1993 times higher than that of the Pt-T300 benchmark. The enhanced performance is attributed to efficient charge carrier separation driven by the interfacial Ti-O-C bond, which optimizes the band alignment between TiO 2 and sp 2 -carbon layers. Mechanistic studies verify that the atomic-level interface establishes a rapid electron transfer pathway, yielding an apparent quantum yield of ∼8.4 % at 420 nm. This work not only establishes a methodology for converting carbohydrates into tailored carbon nanostructures but also develops a novel Ti-O-C bridged TiO 2 @carbon heterojunction architecture, offering a novel approach for designing high-efficiency solar-driven hydrogen production systems.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Lizhen Lian,Min Zhang,Liqiang Wang,You-Nian Liu
Gas–liquid–solid catalytic hydrogenation over carbon-supported catalysts is typically performed at elevated temperatures and high hydrogen pressures, primarily because hydrogen is poorly soluble in the liquid phase. Enhancing the H 2 affinity of catalysts, thereby increasing the surface coverage of active hydrogen species, is an effective strategy; however, it remains challenging. Herein, we demonstrate that the H 2 affinity of carbon-supported catalysts can be optimized by introducing metal oxides into the carbon support, thereby increasing the surface hydrogen coverage on carbon-supported catalysts and ultimately enhancing their hydrogenation performance. As a proof of concept, cobalt supported on a homogeneous composite of d-Al 2 O 3 and N-doped carbon (Co/Al 2 O 3 –NC) has been prepared. The d-Al 2 O 3 component, possessing high H 2 affinity, promotes local H 2 concentration and stabilizes the dissociated hydrogen through the formation of O–H δ+ and Al–H δ- . Consequently, Co/Al 2 O 3 –NC exhibits significantly enhanced hydrogenation performance (TOF = 343 h −1 ) across hydrogenation of p -chloronitrobenzene compared to those of Co/NC (TOF = 32 h −1 ) and Co/Al 2 O 3 (TOF = 53 h −1 ) catalysts under 100 °C and 5 bar H 2 . These findings provide new insights for designing efficient catalysts for gas–liquid–solid catalytic hydrogenation reactions over carbon-supported catalysts.
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产品关联
DOI
高影响因子
Scientific Reports
·
2015
·Vol. 5
·期 1
·17779
·
IF 5.578
Zhao Jia,Yang Linju,McLeod John A.,Liu Lijia
A nominal GeO x (x ≤ 2) compound contains mixtures of Ge, Ge suboxides and GeO 2 , but the detailed composition and crystallinity could vary from material to material. In this study, we synthesize GeO x nanoparticles by chemical reduction of GeO 2 and comparatively investigate the freshly prepared sample and the sample exposed to ambient conditions. Although both compounds are nominally GeO x , they exhibit different X-ray diffraction patterns. X-ray absorption fine structure (XAFS) is utilized to analyse the detailed structure of GeO x . We find that the two initial GeO x compounds have entirely different compositions: the fresh GeO x contains large amorphous Ge clusters connected by GeO x , while after air exposure; the Ge clusters are replaced by a GeO 2 -GeO x composite. In addition, the two GeO x products undergo different structural rearrangement under H 2 annealing, producing different intermediate phases before ultimately turning into metallic Ge. In the fresh GeO x , the amorphous Ge remains stable, with the GeO x being gradually reduced to Ge, leading to a final structure of crystalline Ge grains connected by GeO x . The air-exposed GeO x on the other hand, undergoes a GeO 2 →GeO x →Ge transition, in which H 2 induces the creation of oxygen vacancies at intermediate stage. A complete removal of oxides occurs at high temperature.
研究领域:
材料科学
·
纳米技术
·
固态化学
·
电子结构
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DOI
高影响因子
Reaction Chemistry & Engineering
·
2026
·
IF 2.9
Yuxia Li,Tingting Ge,Zehao Jing,Yanxia Zheng,Yuchao Li,Ming Wang,Haofei Huang,Cuncun Zuo
Tricyclodecanemonoaldehyde (TCDMA) and tricyclodecanedialdehyde (TCDDA) are key intermediates in fine chemicals and are typically synthesized via hydroformylation of dicyclopentadiene (DCPD). However, developing cost-effective and highly active catalysts with high selectivity remains a significant challenge. A series of M-doped CoO catalysts (M = Ag, Cu, Fe, Ni) are synthesized via a co-precipitation method for DCPD hydroformylation, and Ag is identified as the optimal dopant for synergistic regulation of CoO catalytic performance. The structure–activity relationships of the catalysts are systematically elucidated using a combination of characterization techniques, including XRD, SEM/TEM, in situ FTIR, H2-TPD, H2-TPR, and CO-TPR, and the reaction conditions (temperature, catalyst dosage, pressure, and time) are systematically optimized. Under the optimal reaction conditions (150 °C, 7 MPa, 24 h), the 10% Ag/CoO catalyst achieves a DCPD conversion of 72%, a total aldehyde selectivity of 90%, and a combined yield of TCDMA + TCDDA of over 65%. The introduction of Ag nanoparticles not only modulates the surface electronic structure of CoO to promote H2 adsorption and activation but also suppresses the excessive reduction and aggregation of cobalt active species during the reaction, thereby enhancing both catalytic activity and structural stability. Based on experimental characterization and performance evaluation, a dynamic catalytic cycle mechanism for DCPD hydroformylation on the Ag/CoO surface is proposed, clarifying the synergistic catalytic effects of Ag and CoO active sites. Compared with traditional precious metal catalysts, the Ag/CoO bimetallic catalyst features low cost, simple preparation, and excellent catalytic performance and exhibits significant potential for industrial application in the green synthesis of TCDMA and TCDDA.
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BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
·
2019
·Vol. 92
·期 6
·1047-1052
·
IF 4.431
Jiang Jifei,Zhu Qiong,Guo Yu,Cheng Lin,Lou Yongbing,Chen Jinxi
Photocatalytic hydrogen production is an effective strategy for meeting energy challenges. Here, a composite for photocatalytic hydrogen production via introduction of UiO-66 nanospheres into flower-shaped ZnIn2S4 microspheres (ZIS/U6) is described. The optimum composite with 20 mg UiO-66 loading displayed the high photocatalytic rate of 1860.9 µmol g−1 h−1 with an apparent quantum efficiency of 1.4% at 420 nm under visible-light irradiation, which is nearly 3 times higher than that of ZnIn2S4. The improved photocatalytic H2 rate mainly benefited from effective electron transfer between ZnIn2S4 and UiO-66. Additionally, we tried to introduce UiO-66-NH2 and UiO-66-(SH)2 with excellent visible light absorption into ZnIn2S4 to obtain composites. Surprisingly, they did not exhibit better photocatalytic hydrogen production rates. Combined with the electrochemical test results, it was found that they had completely different electron transfer paths from ZIS/U6. Therefore, a different photocatalytic mechanism was proposed and further verified by transient photocurrent.
研究领域:
材料科学
·
化学
·
能源科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）