APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Kai Dai,Taiping Hu,Jinfeng Zhang,Luhua Lu
Cadmium sulfide (CdS), as a promising candidate for photocatalytic hydrogen evolution (PHE), has been widely studied in recent years. However, the PHE performance of CdS is largely limited by the severe photocorrosion and low quantum efficiency. Herein, we reported multi-walled carbon nanotubes (MWCNTs) exfoliated porous reduced graphene oxide (PRGO)-supported inorganic-organic CdS-diethylenetriamine (DETA) hybrid, and the system is designed and prepared to adjust electronic structure and control photocorrosion property. Irradiated by visible light (λ > 400 nm), this novel PRGO/CdS-DETA system exhibits advanced PHE performance of 10.5 mmol g −1 h −1 and apparent quantum efficiency is 29.5% with enhanced photostability. This result is 13.1, 3.9, 1.5 and 1.3 times higher than CdS nanoparticles, CdS-DETA hybrids, MWCNT/CdS-DETA and RGO/CdS-DETA composites. More importantly, the special connection between PRGO and CdS-DETA facilitates the charge carriers separation and large BET specific surface area ( S BET ) boost the PHE of CdS-DETA. Density functional theory (DFT) calculation further confirms the high mobility for charge transport route from CdS-DETA to PRGO. The PRGO/CdS-DETA system photocatalyst with high PHE performance may provide a new insight into photocatalytic material design.
研究领域:
材料科学
·
能源化学
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Nanoscale Advances
·
2021
·Vol. 3
·期 8
·2280-2286
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IF 4.553
Honglei Wang,Shengyang Tao
Rational optimization of the surface electronic states and physical structures of non-noble metal nanomaterials is essential to improve their electrocatalytic performance. Herein, we report a facile dual-regulation strategy to fabricate NiFeP/Ni (P-NiFeP/Ni) porous nanoflowers, which involves Fe-doping and creating pores on nanosheets. The as-prepared P-NiFeP/Ni has a hierarchically porous surface, which exposes more electrochemically active sites and dramatically enhances the electron transfer rate. Thus, it exhibits excellent catalytic activity in both anodic hydrazine oxidation reaction (HzOR) and cathodic hydrogen evolution reaction (HER). Interestingly, the coupled electrolysis cell only offers a potential of 0.162 V at 10 mA cm−2 to enable HzOR boosted H2 evolution, highlighting an energy-saving hydrogen evolution strategy.
研究领域:
材料科学
·
电化学
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Small
·
2025
·
IF 12.1
Bochuan Chen,Yuandong Yan,Shicheng Yan,Zhigang Zou
Water electrolysis faces critical efficiency and cost challenges, primarily due to the high energy demand and low economic value of the oxygen evolution reaction (OER). To overcome this limitation, we introduce an innovative electrochemical-chemical sequential strategy that replaces OER with methanol oxidation (MOR). Our decoupled process comprises cathodic hydrogen evolution reaction (HER) paired with anodic Ni(OH) 2 oxidation to NiOOH in 1 M KOH electrolyte, followed by spontaneous NiOOH reduction via MOR, selectively generating formic acid (HCOOH) with 95% formic acid Faraday efficiency in neutral electrolyte. Crucially, we developed a scalable bottom-up method to electrochemically prepare the active NiOOH catalyst directly from Ni(OH) 2 particles. This catalyst achieved a HCOOH yield of 48.25 mmol per kg catalyst. Collectively, this strategy establishes an efficient and recyclable pathway for alkaline hydrogen production integrated with high-value formic acid synthesis in neutral media.
研究领域:
电化学
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能量转换
·
催化
·
可持续化学
·
氢气生产
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Jihui Yao,Lijuan Su,Lipeng Guo,Xing Wu,Haibo Zhu
N -ethylcarbazole, as a liquid organic hydrogen carrier, has shown great promise in the field of hydrogen storage technology. The development of efficient and stable catalyst for producing H 2 through N -ethylcarbazole dehydrogenation is crucial for its practical application. In this study, a series of mesoporous Al 2 O 3 -supported Pt catalysts with K modification were developed for N -ethylcarbazole dehydrogenation. These catalysts were characterization using various techniques including XRD, N 2 adsorption–desorption, TEM, 27 Al MAS NMR, XPS, NH 3 -TPD, H 2 -TPR, CO-FTIR, and Py-IR, providing detailed structural information to elucidate the structure–activity relationship. Mesoporous Al 2 O 3 was found to possess significant amounts of coordinatively unsaturated pentacoordinate Al 3+ , which greatly promotes the dispersion of Pt species for the formation of small Pt particles. The addition of K was observed to modulate the electronic structure of Pt, reduce the acidity of the catalysts, and inhibit the sintering of Pt. These synergetic effects led to Pt 3.0 /K 3.0 -Al 2 O 3 -m achieving remarkable performance in dodecahydro- N -ethylcarbazole dehydrogenation at 180 °C and 101 kPa, delivering a dodecahydro- N -ethylcarbazole conversion of 100 %, H 2 release amount of 5.63 wt% and dehydrogenation efficiency of 97.10 %. Additionally, this catalyst demonstrated high efficiency in the dehydrogenation of dodecahydro- N -propylcarbazole, octahydro-2-methylindole, and octahydro-1,2-dimethylindole, achieving dehydrogenation efficiencies of 99.60 %, 100 % and 100 %, respectively. These findings provide valuable knowledge for the rational design of efficient metal-based catalysts for liquid organic hydrogen carriers in hydrogen storage systems.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Zhongmin Feng,Zheng Wang,Li-hua Qi,Sijie Yun,Chuang Zu,Ling Huang,Shengping Wang,Huanting Wang
Gas separation using metal organic framework (MOF) membranes has attracted considerable attention in recent years. Despite the progress made, establishing thin, defect-free MOF layers within the porous polymer remains a significant challenge. In this study, a novel approach is reported for the preparation of ZIF-8/Polyethersulfone (ZIF-8/PES) composite membranes via non-solvent-induced phase separation (NIPS)-triggered in-situ crystallization strategy. In this method, PES serves as a solid solvent for Zn(NO 3 ) 2 . During the NIPS process, an asymmetric PES membrane with a skin layer, finger-like pores, and interconnected foam structures is formed. Concurrently, Zn(NO 3 ) 2 diffuses to the skin layer and reacts with 2-methylimidazole (2-MIM), yielding a dense ZIF-8 layer on the PES surface. The simultaneous nucleation and growth of ZIF-8 within the polymer create strong interfacial interactions at the organic-inorganic interface. These interactions improve the compatibility between ZIF-8 and the polymer matrix, reduce interfacial defects. As a result, the composite membrane exhibits enhanced mechanical stability. When the crystallization time is extended to 48 h, the thickness of the ZIF-8 layer reaches approximately 540 nm, and the membrane exhibits an H 2 /CO 2 selectivity of 72.3 ± 3.35 at 298 K. This study provides a facile and effective route for constructing thin MOF membranes on polymeric matrix for high-performance gas separation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Chenxi Shang,Changtai Xu,Boxuan Lu,Shuyi Shang,Tayirjan Taylor Isimjan,Jingya Guo,Xiulin Yang
Developing high-efficiency and stable catalysts for NaBH 4 hydrolysis is critical for safe, high-density and on-demand hydrogen generation. Herein, a core-shell structured Co@SiO 2 @C composite was fabricated as support to immobilize Ru nanoparticles, which precisely regulates electron-metal-support interactions (EMSI). The SiO 2 layer inhibits Ru aggregation and carbon layer accelerates electron transfer, synergistically optimizing Ru electron density and boosting Co–Ru dual active sites. The composite catalyst Co@SiO 2 @C–Ru exhibits significantly enhanced catalytic performance, achieving a hydrogen production rate of 7783.2 mL min −1 g −1 at 25 °C, substantially surpassing most previously reported catalysts. Furthermore, the catalyst retains excellent catalytic activity after five cycles, demonstrating favorable structural and performance stability. Mechanism studies confirm that EMSI drives electron transfer from Co to Ru, optimizing BH 4 – adsorption and activation via Michaelis–Menten kinetics. This work offers a facile strategy for constructing high-performance dual-metal core-shell hydrolysis catalysts.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124637
·
IF 7.5
Qiushuo Hu,Xinle Wang,Fengxia Tong,Xizhuang Liang,Dujuan Dai,Xiaolei Bao,Jianxun Qiu
Photocatalytic reforming of polylactic acid (PLA) plastic into green hydrogen (H 2 ) and high-value chemicals provides a promising approach for addressing environmental and energy issues. However, the rational design of high-performance photocatalysts remains a critical challenge. Herein, a novel NiS/ZnIn 2 S 4 (NS/ZIS) Schottky heterojunction is prepared through the uniform decoration of ZnIn 2 S 4 nanosheets with amorphous NiS. Mechanism studies reveal that the construction of Schottky barrier promotes the electrons transfer from ZnIn 2 S 4 to NiS, achieving efficient H 2 evolution. The photogenerated holes remaining on the surface of ZnIn 2 S 4 possess moderate oxidation activity, which can enable efficient and selective catalytic conversion of waste plastics to pyruvic acid (PA). Consequently, the NS/ZIS composite exhibits outstanding visible-light-driven generation rates of H 2 and PA, reaching 3.81 mmol g −1 h −1 and 2.95 mmol g −1 h −1 , respectively. These values are 4.6-fold and 2.3-fold as high as those acquired from pristine ZnIn 2 S 4 . It also achieves a PA selectivity of 80.6% and an apparent quantum yield of 10.3% at 420 nm. Moreover, the NS/ZIS thin film synthesized via drop-casting has prominent H 2 evolution activity and PA selectivity under natural sunlight exposure, which manifests its promising prospect in practical industrial utilization. This work presents a feasible method for converting waste plastic into H 2 and value-added chemicals, thereby contributing to the mitigation of escalating white pollution.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 31
·42546-42556
·
IF 7.8
Liu Yingjie,Chen Song,Zu Bingqian,Bao Liping,Liu Tian,Chi Jian,Chen Jilong,Zhou Jingtao,Wu Liang
Solar-driven photoreforming of plastic waste into hydrogen offers a promising solution to simultaneously address environmental pollution and sustainable fuel production. However, developing efficient visible-light photocatalysts that couple plastic oxidation with proton reduction for green H 2 generation is still a challenge. Herein, a series of Zn x Cd 1- x S (ZCS) nanoplates (NPs) is rationally synthesized via a cation exchange strategy with Cu 1.8 S NPs serving as sacrificial templates and used for efficient evolution of H 2 from waste plastic. Among these, ZCS-5 NPs achieve an optimal balance between visible-light absorption and redox driving force, delivering a high hydrogen evolution rate of 39.81 mol g –1 h –1 under visible light, outperforming their binary CdS and ZnS NPs. Notably, ZCS-5 NPs also enabled efficient photoreforming of plastic substrates, achieving H 2 evolution rates of 14.98 and 2.28 mol g –1 h –1 from polylactic acid and polyethylene terephthalate under mild aqueous conditions, respectively. Overall, this work presents a potential approach for solar-driven plastic upcycling and green hydrogen generation.
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Haoyi Guo,Pan Cao,Muxian Liu,Guohui Dai,Bei Liu,Changyu Sun,Chun Deng,Guangjin Chen
Hydrogen is regarded as a promising alternative to fossil fuels; however, approximately 95% of the global hydrogen supply still comes from “gray hydrogen”, with high carbon emissions. Efficient separation of CO2 and H2 is a key challenge in gray hydrogen production. This study proposes a novel H2 recovery process based on an aqueous solution of 2-methylimidazole (2-MeIm). The 2-MeIm aqueous solution possesses both strong CO2 absorption capacity and easy desorption performance, which can reduce energy consumption. Pure component solubility experiments were carried out at temperatures ranging from 283.15 to 353.15 K and pressures ranging from 0 to 2.0 MPa, yielding 66 sets of pure CO2 solubility data and 15 sets of pure H2 solubility data, which were used to regress the binary interaction parameters of the NRTL model. Comparison between the fitted NRTL model parameters and the experimental data indicates that the mean relative error of CO2 is 5.19%, whereas that of H2 is only 0.18%. Further, single-equilibrium-stage phase equilibrium experiments were conducted using a mixed gas stream with a CO2/H2 molar ratio of 40:60 to further validate the accuracy of the fitted NRTL parameters. The results demonstrate that the solubility-based fitted model achieves a mean absolute error (MAE) of 0.03 for gaseous CO2 and a mean relative error (MRE) of 0.93% for liquid-phase CO2, indicating high predictive accuracy. Based on Aspen Plus, this study has developed a rigorous process simulation model with a processing capacity of 100,000 N m3/h. The operating conditions were defined through sensitivity analysis, resulting in the following optimized parameters: 7 theoretical stages for the absorber, an operating pressure of 3.8 MPa, a volumetric gas-to-liquid ratio of 200, and a desorption temperature of 373.15 K. Under these conditions, H2 purity and recovery reached 99.99% and 99.13%, with specific energy consumption of only 260.27 kgoe/t H2 (10.88GJ/t H2). Compared with the conventional Rectisol process, the 2-MeIm-based process not only achieves higher H2 purity and recovery rate, but also significantly reduces total energy consumption by 32.07%. This marked performance enhancement underscores the outstanding energy-saving potential of the 2-MeIm system in the field of H2/CO2 separation.
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Nature Catalysis
·
2026
·
IF 48.3
Wu Huixin,Xiang Qian,Wang Liang,Wang Hai,Luo Qingsong,Lv Yating,Deng Lifan,Wu Yuexin,Hui Yu,Tang Rui,Yuan Wentao,Wang Yong,Wu Qing,Cao Xiao-Ming,Wang Liang,Xiao Feng-Shou
Hydrogenation of pyridines is particularly challenging because their strong coordination to metal sites hinders hydrogen adsorption and can poison the catalysts. Here we show that Ni nanoparticles (NPs) within zeolite crystals can overcome this problem, owing to a network of micropores that features a greater proportion of free Ni sites for hydrogen adsorption even in the presence of pyridines. As a result, a high activity was achieved under mild conditions, substantially outperforming those of the commercial Raney Ni and conventional supported Ni catalysts. In addition, Ni leaching from the Ni NPs within the zeolite crystals was effectively hindered under the reaction conditions, achieving excellent stability. The versatility of the approach was shown by synthesizing Pd NP analogues, which showed improved activity compared with the conventional supported Pd catalysts.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2026
·
IF 4.5
Si Sun,Yijing Zhang,Ming Wang,Youhua Zhao,Zhehua Jia,Shenzhen Cong
Hydrogen (H 2 ) is a key feedstock for clean energy, and efficient separation of H 2 /CO 2 is an important link. To solve classic ZIF-8 membrane difficulties, such as long preparation times and weak binding force between crystals and supports, this work used an innovative gel-assisted in-situ growing approach. Specifically, a zinc-based gel was placed onto the PSf support and thermally activated, resulting in the creation of an ultra-thin dense membrane with a thickness of about 100 nm. The effects of reaction time and 2-MIM concentration on membrane performance were thoroughly examined. The results showed that the 0.8-ZIF-8-40 membrane had the best separation performance. The resulting 0.8-ZIF-8-40 membrane exhibited an H 2 permeance of 2200 GPU and an H 2 /CO 2 selectivity of 33, surpassing the Robeson upper bound (2008). Furthermore, the membrane maintained good separation performance after 60 h of continuous operation.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Yuxin Tang,Xinyi Yang,Lingyu Zeng,Bili Tan,Fei Qi,Bo Feng,Liang Wang,Guangbo Che
Precise atomic-scale interface engineering across the entire pH range remains a formidable challenge for photocatalytic H 2 evolution. Herein, hexamethylenetetramine (HMT) is introduced as a bifunctional surface modifier that spontaneously constructs Pd-N coordination bridges on g-C 3 N 4 . The interfacial Pd-N bonds collectively down-shift the N-p-band center away from the Fermi level, break intrinsic surface charge symmetry of C/N atoms, and fully expose the originally buried N active sites, thereby steering the hydrogen adsorption free energy (|ΔG H* |) toward thermoneutral. Simultaneously, the Pd-N bond confines Pd cluster growth to ∼5 nm, doubling specific surface area and enriching edge active sites that serve as primary proton reduction centers. Transient photoelectric voltage results reveal that the Pd-N electron transfer channel shortens the carrier transfer path and prolongs photoelectron lifetime, enabling quantitative electron delivery under acidic, neutral, and alkaline environments. As a result, the Pd-CN-HMT sample presents an efficient H 2 evolution rate across the entire pH window. This work advances the field by providing a versatile ligand-based strategy to precisely tailor the interfacial electronic structure via strong chemical bonding, offering a distinct and scalable solution for constructing high-performance pH-universal photocatalysts.
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