Molecular Catalysis
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2024
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IF 3.9
Yu Chen,Ming-Yu Qi,Zi-Rong Tang
Integrating selective organic transformation and hydrogen (H 2 ) evolution in one photoredox reaction system is one of the most sustainable and promising approaches to efficiently produce solar fuels and chemicals by simultaneously utilizing photogenerated electrons and holes. Herein, through the cation-exchange engineering method, the nanoleaf-like Pd/CdS composites are gingerly fabricated for visible-light-driven receptor-free dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to 3,4-dihydroisoquinoline (DHIQ) and H 2 under ambient conditions. The optimized electronic structure endows Pd/CdS with a narrow band gap and suitable energy band positions, thus facilitating the light harvesting as well as the separation and transfer of photoexcited charge carriers. Consequently, the Pd/CdS exhibits significantly improved photoredox activity compared to bare CdS . In-situ Fourier-transform infrared spectroscopy and electron paramagnetic resonance spectroscopy track the progression of reaction intermediates during such a dual-functional photoredox-catalyzed system, revealing that the carbon-centered radical is the key reaction intermediate in this reaction process. It is anticipated that this work would guide the rational utilization of CdS-based materials to enable simultaneous photochemical coupling of organic transformation and H 2 evolution.
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PHYSICA B-CONDENSED MATTER
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2026
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IF 3.2
Junyu Huang,Di Lin,Wei Li,Bo Wang,Huiyang Xu,Zimo Wang,Yongyi Li,Shuanglong Li,Xiaorui Huang
The PCN/CdS/CdIn 2 S 4 composites exhibit excellent photocatalytic performance for H 2 evolution, H 2 O 2 production and dye degradation. • Spontaneous interfacial band bending drives a dual Z-scheme pathway to preserve highly active photogenerated charge carriers. • The superoxide radicals (.•O 2 − ) is the primary species for both continuous H 2 O 2 generation and rapid pollutant decomposition. Addressing the escalating global energy and environmental crises demands efficient, sustainable, and robust technologies. In this study, a ternary composite PCN/CdS/CdIn 2 S 4 integrating phosphorus-doped carbon nitride (PCN), cadmium sulfide (CdS), and indium cadmium sulfide (CdIn 2 S 4 ) was rationally designed via a multi-step assembly process. The optimized heterojunction exhibits outstanding performance, achieving remarkable H 2 and H 2 O 2 production rates of 7614 and 6873 μmol∙g −1 h −1 , respectively. Additionally, it demonstrates ultra-fast degradation kinetics, mineralizing 99.4% of methyl orange within just 30 min. Mechanistically, spontaneous interfacial band bending drives a dual Z-scheme charge transfer pathway. This specific energy band alignment effectively preserves strongly reducing electrons and highly oxidizing holes while significantly suppressing charge carrier recombination. Furthermore, radical trapping confirms that superoxide radicals (∙O 2 − ) are the pivotal active species, driving a two-step single-electron reduction pathway (O 2 →∙O 2- →H 2 O 2 ) for continuous H 2 O 2 generation, and coupling synergistically with localized holes for rapid organic pollutant decomposition.
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AICHE JOURNAL
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2026
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IF 4
Zhiheng Wang,Ningning Wu,Jiali Huang,Tuo Ji,Han Lin,Liwen Mu,Xiaohua Lu,Jiahua Zhu
Direct synthesis of hydrogen peroxide (DSHP) from H 2 and O 2 is indeed a promising sustainable alternative to the conventional anthraquinone oxidation process, yet achieving high H 2 O 2 productivity and selectivity simultaneously remains a significant challenge. Herein, we designed a diode-inspired interfacial microenvironment to address this challenge by synchronizing the kinetic relay of the key transport and reaction steps in DSHP. Specifically, this microenvironment was fabricated by grafting hydrophobic silane molecules onto the carbon surface followed by loading palladium nanoparticles. Results indicate that the interfacial microenvironment enables an efficient relay of H 2 dissociation, H 2 O 2 formation and desorption, shutting down the reverse path of the side reaction. Benefiting from this diode-inspired interfacial design, high H 2 O 2 productivity of 21,647.1 mol kg Pd −1 h −1 and H 2 O 2 selectivity of 93.3% were successfully achieved under ambient conditions. This work demonstrated the critical role of the interfacial microenvironment in regulating the synergy between mass transfer and reaction in heterogeneous reaction.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Yanmei Li,Chunjie Chen,Yali Zhao,Wufeng Wu,Yanying Wei,Haihui Wang
Two-dimensional metal–organic framework (MOF) membranes have emerged as competitive candidates for efficient gas separation owing to their ultrashort diffusion pathways and highly tunable nanochannels. However, unavoidable linker rotation within 2D frameworks constrain accurate molecular sieving. Herein, heteroleptic Zn(bim)(OAc) nanosheets are employed for constructing high-performance membranes, where cooperative 2D-3D linkers coupling regulates framework motions. The 3D acetate (OAc − ) linkers limit the amplitude of motion, whereas planar 2D benzimidazolate (bim) linkers introduce locally rotational freedom through weaker M−N coordination bond, generating precise angstrom-level, dynamically tunable pore window. The heteroleptic membrane achieves considerable H 2 /CO 2 selectivity of ∼ 134, surpassing the upper bounds of traditional polymer membranes. This work demonstrates that cooperative 2D-3D linkers coupling provides a feasible pathway to engineer precise, dynamically tunable apertures in 2D MOF nanosheet membranes, offering a promising avenue for designing high-performance membranes.
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Journal of Cleaner Production
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2026
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IF 10.7
Junqi Wang,Xiangjun Liu,Jingjing Ma,Hu Xu,Kuankuan Liu,Yuxin Wei
Transitioning toward sustainable energy systems requires H 2 production routes that are both efficient and environmentally responsible. In this work, biomass-based photocatalytic H 2 production was systematically investigated by integrating catalyst synthesis optimization with environmental assessment. A CdS-based photocatalyst modified with Ti 3 C 2 T x MXene was synthesized via an ultrasound-assisted approach, and the effects of ultrasonication conditions, catalyst loading, and reaction temperature on photocatalytic performance were evaluated. Under optimized conditions, the MXene/CdS photocatalyst achieved a H 2 production rate of 16.212 mmol g −1 ·h −1 with good cycling stability. To assess the environmental implications of different experimental strategies and operating conditions, a cradle-to-gate life cycle assessment was conducted and complemented by outdoor photocatalytic tests under natural sunlight. The results indicate that moderate ultrasonication, appropriate catalyst dosage, and optimized reaction temperature can effectively reduce environmental burdens. Variations in solar availability further influence environmental performance, highlighting the combined importance of process optimization and realistic operating conditions. Overall, this study demonstrates that coupling photocatalytic performance optimization with environmental assessment provides a more comprehensive understanding of the opportunities and limitations of biomass-based H 2 production.
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JOURNAL OF MEMBRANE SCIENCE
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2026
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IF 8.8
Yufei Wang,Borui Hou,Wenbo Li,Zaichao Guo,Jingyi Ma,Yingying Wang,Shuming Li,Wufeng Wu,Zenan Shi,Zong Lu,Li Ding,Huijun Yao,Sheng Dai,Yanying Wei,Haihui Wang
Heavy ion irradiation introduces straight-through channels in MXene membranes. • ∼3 Å pores with narrow size distribution are generated by Fe ion irradiation. • Heavy ion irradiation can penetrate through micron-thick MXene membranes. • Fe ion irradiation enhances H 2 permeance and H 2 /CO 2 selectivity. Two-dimensional (2D) nanosheets are promising for fabricating H 2 sieving membranes due to their atomic-scale thickness, but the tortuous pathways formed by nanosheet stacking limit efficient gas transport. Introducing artificial in-plane pores on 2D nanosheets offers a solution, yet existing methods suffer from broad size distribution with large pore size and shallow pore-forming depth through membranes. Here, we propose a kind of straight-through angstrom-scale channelled MXene nanosheet membranes for H 2 sieving engineered by a heavy ion irradiation strategy. A key advantage of the pore-forming strategy is that selecting specific heavy ion species and energy enables precise control of energy loss, directly guaranteeing ultra-uniform pore size at the angstrom scale. After Fe ion irradiation, the obtained pores penetrating through micron-thick membranes exhibit size of ∼3 Å with narrow distribution (proportion of 87%), high pore density (>10 13 cm −2 ) and uniform distribution simultaneously. The optimal membranes exhibit an H 2 permeance of 1898 GPU, a sixfold increase over the pristine membrane assembled with nonporous MXene nanosheets, while retaining a high H 2 /CO 2 selectivity of ∼91, outperforming most current membranes. This work provides a scalable strategy for pore-engineering of 2D nanosheet membranes, and establishes a robust platform for gas separation, catalysis, and environmental applications. Download: Download high-res image (331KB) Download: Download full-size image
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2026
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IF 9.2
Lanxin He,Zhihan Yu,Quanjun Xiang
Covalent triazine frameworks (CTFs) possess high conjugation and tunable structures for photocatalysis, but low electron-hole separation and poor stability limit their hydrogen evolution from water splitting. Herein, a new S-scheme heterojunction was effectively created through electrostatic self-assembly of a fluorenone-based covalent triazine framework (FOCTF) with heptazine crystalline carbon nitride (HCN). Staggered band structures were confirmed via Mott-Schottky measurements and UPS characterization, and electron spin resonance (ESR) analysis validated the S-scheme electron transfer pathway. The optimal HCN@FOCTF sample exhibited the highest photocatalytic hydrogen production rate (80.79 μmol h −1 ) at 405 nm, with an apparent quantum yield of 32.51%. Experimental studies confirm that HCN@FOCTF exhibits outstanding photocatalytic performance and stability. The constructed S-scheme heterojunction generates a favorable intrinsic electric field, accelerating directional S-scheme charge carrier transport and thereby enhancing carrier separation and utilization rate. This work proposes a novel idea for constructing an S-scheme heterojunction to regulate electron transfer pathways, towards efficient photocatalytic hydrogen production.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2026
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IF 9.2
Jinxing Yu,Ri Han,Shu Jin,Xiaoxiang Xu
BiFeO 3 is a narrow-bandgap semiconductor promising for solar water splitting but is generally subject to a low photocatalytic activity due to the poor separation of photocarriers (e − and h + ). In this work, BiFeO 3 has been combined with BaTiO 3 to form the solid solutions (i.e. (BiFeO 3 ) 1-x (BaTiO 3 ) x (0 ≤ x ≤ 1)) which demonstrate a much-improved activity for photocatalytic H 2 production under visible light illumination. The solid solution strategy not only tunes the bandgap but also modifies the dielectric constant that is critical for a high photocatalytic activity. A high dielectric constant contributes to an improved photocarrier separation condition due to the screening of the Coulomb interactions between photocarriers and between photocarriers and charged defects. This work reveals a useful solid solution strategy to modify the photocatalytic performance and justifies the importance of dielectric properties for photocarrier separation.
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Chemical Science
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2026
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IF 8.1
Wei Wang,Xiaoyang He,Shuai Dong,Jianying Wang,Deli Wu,Zuofeng Chen
The selective electrooxidation of biomass-derived 1,3-propanediol (1,3-PDO) to high-value 3-hydroxypropionic acid (3-HP) offers a sustainable route for chemical synthesis but is severely hindered by competitive C–C bond cleavage and sluggish reaction kinetics. Here, we propose an electronic structure tuning strategy through interfacial engineering, constructing a Pd−Ni(OH)2 heterostructure to enhance the catalytic performance of Pd nanoparticles. The resulting catalyst exhibits exceptional activity toward the 1,3-PDO oxidation reaction (POR) in alkaline media, requiring a low potential of only 0.645 V (vs. RHE) to achieve a current density of 100 mA cm-2 while maintaining a high Faradaic efficiency of ~94.9%. Comprehensive characterizations and density functional theory (DFT) calculations reveal that strong interfacial interaction induces a downshift in the d-band center of Pd. This electronic restructuring optimizes the adsorption energetics of key intermediates, facilitating rapid desorption of 3-HP from active Pd sites and thereby suppressing over-oxidation and carbon backbone degradation. A membrane electrode assembly (MEA) electrolyzer towards POR demonstrates robust stability, retaining Faradaic efficiencies above 90% during continuous operation. Furthermore, we demonstrate an integrated synthesis-energy device by coupling the POR workflow with the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). This hybrid system, powered by the multifunctional Pd−Ni(OH)2 catalyst, enables flexible temporal deployment via a mode-switching scheme between daytime (HER||POR) and nighttime (ORR||POR). Collectively, this work elucidates an effective strategy for selective biomass valorization through electronic structure tailoring, offering an appealing multidimensional solution for sustainable electrochemical synthesis.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Yanxia Wu,Hanbin Jin,Xiaoling Zhou,Lulu Guo,Qingtao Wang
Oxidizing glycerol to produce formate as a substitute for the traditional slow anodic oxygen evolution reaction is an effective strategy to enhance hydrogen production efficiency and reduce associated costs. However, the development of efficient and stable catalysts remains a significant challenge for the glycerol oxidation reaction coupled with water electrolysis. In this study, we synthesized molybdenum-doped Ni 3 Se 2 /NiSe nanomaterials supported on nickel foam using a straightforward one-step hydrothermal method. In a 1 M KOH solution, the Mo 0.2 catalyst exhibited exceptional electrocatalytic oxidation performance. Specifically, during the glycerol oxidation process, it achieved a current density of 10 mA cm −2 at a remarkably low potential of 1.20 V (vs. RHE) and demonstrated good electrochemical stability at a current density of 50 mA cm −2 . Studies indicate that the incorporation of molybdenum atoms modifies the chemical environment of nickel and selenium atoms, which not only enhances the electrocatalytic activity of the catalyst but also improves the stability of the material itself. Additionally, it facilitates the catalytic oxidation of glycerol at the anode while concurrently promoting hydrogen evolution at the cathode, resulting in the efficient simultaneous production of hydrogen and formate.
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APPLIED SURFACE SCIENCE
·
2019
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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
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化学工程
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能源科学
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CHEMICAL ENGINEERING JOURNAL
·
2026
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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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