Small
·
2024
·
IF 13
Xue Ou,Xinrui Chen,Siyu Zhao,Yarong Shi,Junhua Zhang,Min Wu,Arthur J. Ragauskas,Xueping Song,Zhanying Zhang
Carbon dots (CDs) have a wide light absorption range, which are promising candidates for photocatalytic water splitting H 2 evolution, but they show low activity for hydrogen evolution reaction (HER) due to the slow transfer efficiencies of photogenerated carriers. The electron cloud density of photocatalyst is essential for the separation and migration of photogenerated carriers. In this study, the effect mechanism of electron cloud density regulated by the substituents with different electronic effects on the photocatalytic HER of glucose-based CDs is clarified. CDs-SO 3 H and CDs-OH are first obtained by introducing electron-drawing group (─SO 3 H) and electron-donating group (─OH) using a tailoring post-processing strategy. Experimental results show that the H 2 yield catalyzed by CDs-SO 3 H is 89.95 µmol•g −1 in 4 h, which is about four times that of CDs, and 7.4 times that of CDs-OH. The ─SO 3 H induces a much negative energy band and high electron cloud density on CDs edges, promoting the separation and transfer of photogenerated carriers; while the CDs-OH exhibits a high positive charge density and an upward energy band, hindering the surface complexation of electron-hole pairs and HER. This study will provide an insight into the design of CDs catalysts with efficient photocatalytic HER at a molecular level.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Xuan Miao,Xiao Bai,Peng Zhang,Bolong Wang,Shuyan Wang,Yuzhu Yang,Zenggang Lin,Sixia Li,Binbin Wang,Weisheng Liu
Incorporating two-phase heterojunctions with matching band structures represents a promising strategy for developing photocatalysts with enhanced efficiency. This work prefers a novel approach that employs a template-assisted strategy based on a porous structured UCCN@CeO2 0D/2D S-scheme heterojunction. The proposed method aims to improve photocatalytic activity by harnessing the synergistic effects of monodispersed CeO2 nanoparticles and ultrathin N-defect CN nanosheets. The catalyst demonstrates a remarkable photocatalytic hydrogen evolution rate, reaching an impressive value of 5.59 mmol h–1 g–1 when subjected to simulated sunlight irradiation. Furthermore, the photocatalyst maintains a substantial activity level, yielding 2.35 mmol h–1 g–1 under visible light (≥400 nm). The significant improvement in the photocatalytic performance of the UCCN@CeO2 catalyst is attributed to the unique structural design and effective charge separation facilitated by the S-scheme mechanism. Kelvin probe force microscopy, theoretical calculations, and femtosecond transient absorption spectroscopy affirm the efficient charge transportation across the catalyst interface. Additionally, electron spin resonance spectroscopy measurements further support the charge transfer pathway in the S-scheme. This research presents an innovative approach for designing and developing CN-based catalysts featuring S-scheme heterojunctions, aiming to improve their efficiency and practical use in photocatalytic applications.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Han Xue,Hailong Xu,Xuedan Song,Miaomiao Chen,Xinkui Wang,Min Ji,Min Wang
A porous metal–organic framework (MOF)-based frustrated Lewis pairs (FLPs) were prepared via a ligand replacement strategy to generate organic linker defects in zirconium-based MOF (MOF-808), thereby exposing Zr sites as Lewis acid. Due to the rigid features of the MOF skeleton, the unsaturated metal cluster and the adjacent lattice oxygen (Lewis bases) are in sterically hindered positions, which formed FLP sites with efficient H2 activation ability. This porous heterogeneous FLP catalyst [MOF-808-OH (15%)] exhibits high performance styrene hydrogenation to ethylbenzene with 99% yield. The high structural stability and reusability enabled the catalyst to maintain an over 98% activity after five cycles. This work provides a defect modulation strategy to prepare MOF-based solid FLP catalysts.
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SURFACE & COATINGS TECHNOLOGY
·
2024
·
IF 5.3
Tongguo Huo,Dan Zhu,Jianxin Zheng,Yuan Lin,Yu Dai,Jian Wu
This study systematically investigated for the first time the effects of varying the temperature, pressure, C/Si molar ratio, and H 2 /Si molar ratio on β-SiC coatings produced via chemical vapor deposition (CVD) using the SiCl 4 –CH 4 –H 2 –N 2 system. Thermodynamic theoretical calculations were performed using the HSC Chemistry software. The temperature and C/Si molar ratio considerably affected the morphology, phase, and composition of β-SiC coatings. High-quality β-SiC coatings along the (111) crystal plane exhibiting a uniform surface, high density, low roughness, and good crystallinity were successfully synthesized at 1523.15 K and 200 Pa with a C/Si molar ratio of 1.0 and H 2 /Si molar ratio of 6.5. Additionally, when N 2 was used as the dilution gas instead of Ar, the resulting β-SiC coatings demonstrated reduced roughness, fewer free carbon, increased hardness (37.05 GPa vs. 39.19 GPa), enhanced modulus of elasticity (237.26 GPa vs. 264.24 GPa), and superior coating adhesion (16.48 MPa vs. 18.29 MPa).
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jiayi Liu,Yaohui Zhang,Yujie Ban,Weishen Yang
Emissions from the petrochemical industry often contain by-product hydrogen alongside various hydrocarbons, leading to both resource wastage and increased air pollution. The separation of H 2 from these hydrocarbons is thus of considerable economic and environmental importance. Conventional polymer membranes face inherent trade-offs between gas permeability and selectivity. To overcome this limitation, this study introduces a strategy to assemble metal–organic framework (MOF) nanoparticles into a sponge-like architecture on the surface of an ultrathin rubbery polysiloxane membrane, achieved by synergistically harnessing spin-coating-induced centrifugal forces and polymer–MOF chemical pinning forces. The resulting intricate sponge-like structure greatly promotes repeated adsorption–desorption cycles for the more condensable hydrocarbons, thereby markedly slowing their permeation through the membrane. The composite membrane achieves H 2 /CH 4 , H 2 /C 2 H 6 , and H 2 /C 3 H 8 separation factors of 136, 1370, and 1610, respectively, while maintaining H 2 permeances of 439 to 473 GPU. The membrane's effectiveness is further demonstrated for hydrogen separation from a simulated hydrocarbon-rich industrial tail gas: H 2 is enriched from 10% to 83% in the permeate. In doing so, the membrane not only efficiently recovers hydrogen but also reduce the combined emissions of six representative C 1 –C 4 hydrocarbons by 78%. This sponge-like MOF-polymer composite introduces a new paradigm for advanced H 2 /hydrocarbon separation membranes.
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Nanoscale
·
2025
·
IF 5.1
Wei Zhao,Yuxiang Yang,Yanbin Li,Yimin Liu,Yuezhou Wei,Xinpeng Wang,Deqian Zeng
The advancement of efficient photocatalysts is essential for tackling global energy and environmental issues. In this work, a unique sheet-on-sheet Cd(OH)2/CdS photocatalyst was synthesized via a facile solution strategy, demonstrating significantly improved photocatalytic performance for H2 generation and Cr(VI) reduction. The optimal 5% Cd(OH)2/CdS obtained an impressive H2 production rate of 3475 μmol·g-1·h-1 under visible light, marking a 6.3 times increase compared to CdS. Additionally, the kinetics of Cr(VI) reduction were markedly accelerated, with a rate constant of 0.2803 min-1, representing a 5.7 times improvement over pure CdS. Moreover, the 2D/2D Cd(OH)2/CdS photocatalyst exhibited exceptional stability, maintaining high photocatalytic activity over multiple reaction cycles. Experimental findings and DFT calculations revealed the charge transfer mechanism between CdS nanosheets and Cd(OH)2 cocatalyst. This work provides insights into designing high-performance CdS-based nanophotocatalysts for water splitting and environmental remediation.
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Catalysts
·
2025
·Vol. 15
·期 7
·694
·
IF 4
Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang
The development of non-noble metal catalysts for gas-phase propylene epoxidation with H2/O2remains challenging due to their inadequate activity and stability. Herein, we report a Cs+-modified Ni/TS-1 catalyst (9%Ni-Cs/TS-1), which exhibits unprecedented catalytic performance, giving a state-of-the-art PO formation rate of 382.9 gPO·kgcat−1·h−1with 87.8% selectivity at 200 °C. The catalyst stability was sustainable for 150 h, far surpassing reported Ni-based catalysts. Ni/TS-1 exhibited low catalytic activity. However, the Cs modification significantly enhanced the performance of Ni/TS-1. Furthermore, the intrinsic reason for the enhanced performance was elucidated by multiple techniques such as XPS, N2physisorption, TEM,29Si NMR, NH3-TPD-MS, UV–vis, and so on. The findings indicated that the incorporation of Cs+markedly boosted the reduction of Ni, enhanced Ni0formation, strengthened Ni-Ti interactions, reduced acid sites to inhibit PO isomerization, improved the dispersion of Ni nanoparticles, reduced particle size, and improved the hydrophobicity of Ni/TS-1 to facilitate propylene adsorption/PO desorption. The 9%Ni-Cs/TS-1 catalyst demonstrated exceptional performance characterized by a low cost, high activity, and long-term stability, offering a viable alternative to Au-based systems.
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ENERGY & FUELS
·
2025
·
IF 5.3
Shengqi Lin,Hailong Huang,Jieyi Fan,Chunhe Li,Kuankuan Ren,Weidong Dou
Photocatalytic conversion of biomass-derived compounds into value-added chemicals coupled with hydrogen production presents a promising strategy to address energy and environmental challenges. In this study, a series of NiB/ZnIn2S4 nanocomposites were synthesized via a facile two-step hydrothermal approach. The designed system enables the simultaneous utilization of photoexcited electrons and holes in redox reactions, achieving efficient benzyl alcohol oxidation and hydrogen evolution. The optimized 3%-NiB/ZnIn2S4 nanocomposite demonstrates exceptional photocatalytic performance, exhibiting a hydrogen evolution rate of 7223.2 μmol g–1 h–1 in 1.50 vol % benzyl alcohol solution, representing 2889.3-fold and 4.8-fold enhancements over pristine NiB and ZnIn2S4, respectively. Furthermore, the system maintains robust stability over 14 photocatalytic cycles, achieving 71.7% conversion efficiency and 86.8% selectivity toward benzaldehyde production. The enhanced performance originates from the formation of Z-scheme heterojunctions between NiB and ZnIn2S4, which facilitates efficient charge carrier separation and transport, as evidenced by improved photocurrent response and reduced electrochemical impedance. This work provides valuable insights into the photocatalytic valorization of biomass-derived platform chemicals under visible light irradiation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jun-Qing Ye,Bin Cheng,Yunfei Bu,Jun-Feng Qian,Qian Liang,Ming-Yang He,Qun Chen
The development of high-efficiency photocatalysts for water splitting to hydrogen (H 2 ) is crucial for alleviating energy crisis and environmental problems. In this study, a novel type-II ternary heterojunction photocatalyst, CDs/NH 2 -MIL-125 (Ti)/Cu 2 O, was fabricated through the integration of NH 2 -MIL-125 (Ti) with Cu 2 O and carbon dots (CDs), exhibited excellent photocatalytic H 2 production rate of 12817.1 μmol/g/h with apparent quantum efficiency (AQE) of 17.13 % under visible light irradiation. Characterization revealed a uniform and dense structural integration with a high Brunauer-Emmett-Teller (BET) surface area of 275.9 m 2 g −1 and a suitable energy band gap of 2.18 eV. Furthermore, the heterostructures promoted efficient photo-generated carrier separation and enhanced reduction capabilities . Notably, CDs, serving as cocatalysts or electron acceptors, improved visible light utilization and electron migration, significantly boosting H 2 production. Insights from electron spin resonance (ESR) and density functional theory (DFT) calculations supported the migration mechanisms of electrons. This work presents a significant advance in photocatalytic technology for sustainable energy by designing high-performance CDs-modified heterojunction photocatalysts.
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Molecular Catalysis
·
2024
·
IF 3.9
Fukun Li,Ronghe Yang,Jinhang Dai,Hanyue Deng,Junjun Shi,Wucheng Xie,Juanhua Kong,Tingwang Guo
Biomass upgrading, which supplies important biomaterials, chemicals and fuels, is considered as an efficient way to realize the goal of carbon neutralization. Recently, γ-valerolactone (GVL) has gained increasing attention due to its wide applications. In this work, a novel protocol of microwave-assisted cascade catalytic upgrading of α-angelicalactone (α-AL) to GVL over metal triflate using alcohol as the hydrogen donor was proposed. The yield of GVL production from α-AL upgrading is strongly influenced by the Lewis acid strength of the metal triflate and the reduction potential of the employed alcohol. Among all tests, Sc (OTf) 3 showed the best catalytic performance in isopropanol media, giving 96.4 % GVL yield and 100 % α-AL conversion at 433 K within 3.0 h. Meanwhile, kinetic study indicated transfer hydrogenation of isopropyl levulinate to isopropyl 4-hydroxyvalerate was the rate-limited step with the apparent activation energy of 94.5 kJ/mol. This Sc (OTf) 3 catalyst was highly stable and could be reused for five cycles by simple vacuum distillation. In a word, this work provides an alternative for GVL production from biomass upgrading.
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Catalysts
·
2025
·Vol. 15
·期 6
·544
·
IF 4
Tingting Hu,Baozeng Ren,Liang Zhao
Hydrogen peroxide (H2O2) is an important industrial chemical that is widely applied in many areas. The direct synthesis of H2O2from H2and O2has proved to be a green and economic pathway. Pd-based bimetallic catalysts, due to their superior catalytic performances in this reaction, have attracted intensive attention. Herein, Tetrakis(hydroxymethyl)phosphonium chloride (THPC) was adopted as the protective ligand to immobilize Pd-Au alloy nanoparticles onto activated carbon (AC). The varied Pd/Au molar ratios demonstrated homogeneously distributed Pd-Au nanoalloys with average particle sizes ranging from 3.51 to 5.75 nm. The optimal ratio was observed over the Pd3Au1/AC-THPC catalyst with a maximum H2O2productivity of 165 mol/(kgPd·h) and selectivity of 82.3% under ambient pressure. The relationship between the electronic structure and catalytic activity indicated Pd0was the active site, while the presence of Au inhibited H2O2degradation rate. This research could help in the design efficient bimetallic catalysts for the direct synthesis of H2O2.
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Catalysts
·
2025
·Vol. 15
·期 11
·1032
·
IF 4
Jingmo Zhou,Chaoyue Liu,Wenke Zhao,Faizan Ahmad,Yaning Zhang
This study pioneers the application of metal-doped Fe-Al as multifunctional redox catalysts for tunable syngas production from plastics via a microwave-assisted process (CLG). We rationally designed a series of redox catalysts (Ni, Ca, Ce, Sr, Co) to unlock efficient H2-rich syngas production from (high-density polyethylene) HDPE. A class of metal-doping (Ni, Ca, Ce, Sr, and Co) Fe-Al redox catalysts was engineered, with Ni-doped Fe-Al (Ni-Fe-Al) exhibiting the excellent H2-rich syngas production (75.32 mmol/gHDPE syngas, 47.09 mmol/gHDPE H2). This is attributed to the improved redox activity, which facilitates efficient lattice oxygen transfer and catalytic reforming reactions, alongside improved microwave absorption and a porous structure that promotes reactant access. This strategic material design, coupled with process parameter optimization (800 W, redox catalyst/plastic = 2.0), developed a highly efficient HDPE-to-syngas conversion system. The process produced a high-quality syngas (90.03% H2+ CO, H2/CO ratio = 2.27) with a rapid heating rate (233.0 °C/min) and minimal energy input (3.52 kWh/molgas). This work provides not just an effective upcycling route for plastics, but a fundamental blueprint for designing advanced redox catalysts to unlock the full potential of microwave-CLG.
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