JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Wei Shao,Ying-Wu Zhou,Zhen Chen,Yi-Le Chen,Yi Li,Yu-Jie Ban,Wei-Shen Yang,Ming Xue,Xiao-Ming Chen
Metal-Organic Framework (MOF) membranes act as selective layers have offered unprecedented opportunities for energy-efficient and cost-effective gas separation. Searching for the green and sustainable synthesis method of dense MOF membrane has received huge attention in both academia and industry. In this work, we demonstrate an in situ electrochemical potential-induced synthesis strategy to aqueously fabricate Metal Azolate Framework-4 (MAF-4) membranes on polypropylene (PP) support. The constant potential can induce the heterogeneous nucleation and growth of MAF-4, resulting an ultrathin membrane with the thickness of only 390 nm. This high-quality membrane exhibits a high H 2 /CO 2 separation performance with the H 2 permeance as high as 1565.75 GPU and selectivity of 11.6. The deployment of this environment friendly one-step fabrication method under mild reaction conditions, such as low-cost polymer substrate, water instead of organic solvent, room temperature and ambient pressure shows great promise for the scale-up of MOF membranes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Ligang Ma,Chao Lin,Wenjun Jiang,Le Xu,Yujie Shao,Tianyu Zhu,Ting Zhao,Xiaoqian Ai,Xiaoshan Wu
In the face of energy scarcity and environmental degradation, photocatalysis emerges as a green and highly efficient method to convert solar energy into a renewable energy source . In this study, CdS nanoparticles were successfully grown in situ along the edges of ZnIn 2 S 4 nanosheets using ultrasound during the synthesis process and the second phase precipitation of In(OH) 3 appeared in the process of preparation. Optimal Cd and S ratios resulted in ZnIn 2 S 4 @In(OH) 3 @CdS heterojunction exhibiting remarkable photocatalytic H 2 production performance compared to standalone ZnIn 2 S 4 and CdS. The internal heterojunction interface within the composite naturally generates an electric field, enhancing carrier separation and facilitating their transport. Additionally, the inclusion of In(OH) 3 further expedites carrier extraction. Ultimately, the mechanism behind the photocatalytic H 2 production was elucidated using the Z-scheme mechanism. This work introduced a novel approach to fabricating multifunctional photocatalysts , presenting a fresh perspective in their design and preparation.
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CATALYSIS TODAY
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2024
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IF 5.2
Jiaxin Zheng,Miao Wang,Xinli Tong,Ye Yuan
The catalytic selective etherification of 5-hydroxymethyl furfural (5-HMF) is considered as a feasible route to prepare the biofuels from biomass feedstocks. In this work, a novel solid acid catalyst derived from the flower-like MoS 2 is synthesized by combination of the facile hydrothermal method and reduction process. Therein, the number of Lewis and Bronsted acidic sites derived from the exposed Mo edges of MoS 2 can be efficiently regulated by changing the hydrogen annealing conditions. The prepared MoS 2 -450-R catalyst exhibited a prominent activity for the conversion of 5-HMF to 5-(methoxymethyl)furanal dimethyl acetal (5-MFDMA) through the tandem acetalization and etherification under N 2 atmosphere, in which a 99.0 % conversion with 83.7 % selectivity of 5-MFDMA is obtained. Further investigations revealed that the abundant acidic sites of MoS 2 -450-R plays a crucial role on the reaction of 5-HMF with methanol. Finally, based on the characterization of catalyst and reaction phenomena, a possible reaction network for the acetalization and etherification of 5-HMF with the methanol has been proposed.
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Small
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2024
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IF 13
Yang Ming,Zhixing Cheng,Shuo Shi,Jing Su,Weng-Fu Io,Hanbai Wu,Jiashen Li,Bin Fei
Nanoarchitectonics of semiconductors shed light on efficient photocatalytic hydrogen evolution by precisely controlling the surface microenvironment of cocatalysts. Taking cadmium zinc sulfide (CZS) nanoparticles as a target, the spontaneous modifications are conducted by interactions between surface Cd 2+ /Zn 2+ atoms and thiol groups in thioglycolic acid. The capping ligand impacts the semiconductor surface with a negative electronic environment, contributing to the full coverage of CZS by nickel-cobalt hydroxides (NiCo-LDHs) cocatalysts. The obtained core-shell CZS@NiCo-LDHs, possessing a shell thickness of ≈20 nm, exhibits a distinguished topology (S BET = 87.65m 2 g −1 ), long surface carrier lifetime, and efficient charge-hole separation. Further photocatalytic hydrogen evaluation demonstrates an enhanced H 2 evolution rate of 18.75 mmol g −1 h −1 with an apparent quantum efficiency of 16.3% at 420 nm. The recorded catalytic performance of the core-shell sample is 44.6 times higher than that of pure CZS nanospheres under visible light irradiation. Further density functional theory simulations indicate that sulfur atoms play the role of charge acceptor and surface Ni/Co atoms are electron donors, as well as a built-in electric field effect can be established. Altogether, this work takes advantage of strong S affinity from surface metal atoms, revealing the interfacial engineering toward improved visible-light-driven photocatalytic hydrogen evolution (PHE) activity.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yonggang Lei,Kim Hoong Ng,Yingzhen Zhang,Zengxing Li,Shen Xu,Jianying Huang,Yuekun Lai
In an attempt to construct efficient photocatalytic H 2 production system, designing a practical way to integrate co-catalyst and semiconductor is of great importance for future commercialization. Herein, we report a facile one-pot loading of CdS onto WC through the facile solid–liquid mixing method. The resultant visible light-responsive WC-supported CdS photocatalyst, at different WC wt.%, is assessed in photocatalytic hydrogen production, with lactic acid as an electron donor. Experimental results confirmed the positive effects of WC, with 3 wt% WC-loaded CdS photocatalyst (CdS/WC) exhibiting the highest hydrogen evolution rate of 9180 μmol h −1 g −1 . Such achievement is associated to 2.1 and 43 folds activity improvements from that of CdS/Pt(3 wt%) and pure CdS photocatalysts, respectively. Meanwhile, an apparent quantum efficiency (AQE) of 14.3% was also recorded by the same photocatalyst from the single-wavelength photocatalytic reaction at 420 nm. All these enhancements can be attributed to the incorporation of WC, which extending and improving the light absorbability of CdS. Concurrently, the adjoining WC also provides rapid electron transfer channel and water reduction site, which facilitate the spatial separation of charges while promoting the kinetics of hydrogen production reactions. This study presents a facile synthesis method for CdS/WC photocatalyst, which offers high reliability for industrial scale hydrogen production.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Feng Ye,Shuanshi Fan,Xuemei Lang,Yanhong Wang,Gang Li
Silicalite-1 zeolite membranes were successfully activated at 300–350 °C in a hydrogen atmosphere. FTIR, TGA, and N 2 adsorption-desorption characterizations confirmed that the amount of the organic structure directing agent (OSDA) residue in silicalite-1 zeolite channels was tunable. The H 2 -calcined membrane showed a lower gas permeance than that of the air-calcined membrane due to the partial pore blockage by the OSDA residue. The permeance of H 2 and CO 2 increased with increasing temperature, showing an activated diffusion-like mechanism. The activation energies for the permeation of H 2 and CO 2 were in the range of 1.63–4.15 and 0.76–5.90 kJ mol −1 , respectively, which confirmed the reduced average membrane pore size and different pore surface chemistry due to the presence of the OSDA residue in the membrane. Significant interactions between CO 2 molecules and OSDA residues confined in the membrane resulted in a notably lower CO 2 permeance compared to N 2 and CH 4 , despite CO 2 having a smaller kinetic diameter. Enhanced H 2 /CO 2 selectivity in the silicalite-1 zeolite membrane, featuring confined OSDA residue, was attributed to the reduction in membrane pore size and the fine-tuning of pore surface chemistry.
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CHEMISTRY OF MATERIALS
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2024
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IF 7.2
Xiangdong Li,Kangchi Zhang,Wentao Liang,Cheng Zhong,Di Mai,Azizur Rahman,Xiaoyu Sun,Rucheng Dai,Zhongping Wang,Qiang Wu,Zengming Zhang
Recently, hydrogen sulfide (H2S) and phosphine (PH3) have attracted great attention since the observation of superconducting transitions with high crucial temperatures under high pressure, which inspired subsequent investigations of the superconductivity of nonmetallic hydrides. Here, we report the successful photochemical and thermal syntheses of a series of novel H2S–PH3–H2 ternary hydrides with varying H2S and PH3 molar ratios. Raman, infrared, UV–visible absorption spectra, and electrical transport measurements are employed to investigate the chemical reaction and electronic structure transformation under high pressure. The pressure-induced polymerization of PH3 can be confirmed in H2S–PH3–H2 by Raman and infrared spectra, and the polymerization product, P4H6, can be recovered to ambient pressure; additionally, the polymerization pressure of PH3 is evidently hampered with increasing H2S concentration. Furthermore, it has been found that low temperatures can significantly inhibit the pressure-induced polymerization of PH3. The formation of Hittorf’s phosphorus is experimentally confirmed upon unloading pressure from 100 GPa to ambient pressure, which strongly implies the decomposition of P4H6 under high pressure. The H2S–PH3–H2 molecule gradually turns red and is eventually opaque following compression, which is consistent with the red shift of the UV–visible absorption spectra. Furthermore, synchrotron infrared absorption spectra and electrical transport examined above 65 GPa indicate the insulator-to-metal transition of H2S–PH3–H2 caused by dehydrogenated polymerization of P4H6 to Hittorf’s phosphorus.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Jiahao Zhao,Xiaohui Ma,Mengyao Ren,Jianlin Zhao,Chunhua Yuan,Jinlong Cui,Wenxiu He
The development of efficient and low-cost photocatalysts has always been sought in H 2 production from water cracking. Herein, a series of MoB/Mn 0.43 Cd 0.57 S composites were developed for high-performance photocatalytic H 2 production. Mn 0.43 Cd 0.57 S nanoparticles were deposited on bulk metalloid MoB via a hydrothermal method (as confirmed by morphology tests) to construct a Schottky heterojunction. In the composites, the Fermi levels of Mn 0.43 Cd 0.57 S and MoB were rearranged (as confirmed by ultraviolet photoelectron spectroscopy) and the electrons of Mn 0.43 Cd 0.57 S rapidly migrated to MoB (as confirmed by X-ray photoelectron spectroscopy). Ultimately, the formation of the Schottky heterojunction significantly improved interfacial carrier separation, leading to efficient H 2 production. MoB, which exhibits a Pt-like electronic structure, provided active sites for H 2 evolution in the heterojunction composites. Furthermore, compared with those of Mn 0.43 Cd 0.57 S, the visible-light absorption capacity and H 2 evolution kinetics of the heterojunction composites were also vastly improved. After photocatalytic H 2 production, the performance of all heterojunction composites markedly increased. The performance of the composite with 20 % MoB/Mn 0.43 Cd 0.57 S) was the highest (4146.92 μmol·g −1 ·h −1 ), which was 11.3 times that of Mn 0.43 Cd 0.57 S (367.56 μmol·g −1 ·h −1 ). The stability of the composites was further evaluated, and the 20MoB/Mn 0.43 Cd 0.57 S composite lost only 12.8 % of its activity, indicating its excellent photostability. The underlying mechanism of H 2 production over the heterojunction composites was also investigated. This work provides an innovative approach for achieving high-efficiency H 2 production in a sulfide solid solution modified by a metalloid MoB cocatalyst.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Haibo Tao,Yan Xia,Tao Tang,Yuan Zhang,Shi Qiu,Junkang Chen,Zhengjiang Xu,Lei Li,Jiajun Qiu,Panfeng Wang,Jianghong Wu,Xiaobing Zhao,Shuogui Xu,Guocheng Wang
Oxidative stress regulation and synchronized promotion of angiogenesis are critical factors in the healing process of diabetic wounds. However, existing research often fails to fully consider the dynamic interplay between these two biological processes and their time-dependent roles in diabetic wound healing. This study innovatively introduces a novel hydrogen (H 2 )-releasing microneedle patch capable of precisely controlling the regulation of oxidative stress and the promotion of angiogenesis through a bidirectional responsive mechanism of microneedles and backing layers. Specifically, we employ ammonia borane (AB)-loaded mesoporous silica nanoparticles (MSN) as a source of H 2 , combined with polyvinyl pyrrolidone (PVP) to fabricate microneedles. This design effectively clears excessive reactive oxygen species (ROS) in deep tissues and promotes the M2 polarization of macrophages. Concurrently, we utilize cobalt-adsorbed graphene oxide (GO/Co 2+ ) mixed with polyvinyl alcohol (PVA) to prepare backing layers, which not only release Co 2+ upon the reduction of oxygen-containing functional groups in GO by H 2 diffused from deep tissues to synergize with H 2 for enhanced vascularization, but also endow the microneedle patch with near-infrared light-responsive antimicrobial properties, crucial for managing diabetic infected wounds. Through this innovative dual-action mechanism, our research significantly accelerates the healing process of infected wounds in a diabetic mouse model. Moreover, single-cell sequencing results further confirm the pivotal role of H 2 in regulating oxidative stress, promoting macrophage M2 polarization, and stimulating angiogenesis. These results not only showcase the unique features of our microneedle patch but also offer new perspectives and therapeutic strategies for the treatment of diabetic wounds.
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FUEL
·
2025
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IF 7.5
Baofang Zhang,Ziyu Zengcai,Wenting Lin,Wenjie Gu,Dizhou Lou,Ruixi Luo,Qingwei Meng,Yunhong Pi,Tiejun Wang
Herein, Cu 2 O/Ti 3 C 2 T x @TiO 2 is designed by facile one-step strategy of glucose oxidation–reduction reaction for efficient H 2 production from the photothermal-driven reforming of methanol solution (PTRM). At 210 °C, the high H 2 production rate of 87404.0 μmol g cat −1 h −1 (apparent quantum efficiency of 20.6 % at 550 nm) over Cu 2 O/Ti 3 C 2 T x @TiO 2 under photothermal-driven condition is roughly 4 times that of the single thermal condition. The excellent photothermal H 2 yield activity over Cu 2 O/Ti 3 C 2 T x @TiO 2 is attributed to effectively separate carriers and reduced activation energy due to the synergistic effect of light and heat (55.05 kJ·mol −1 ) comparing to pure thermal condition (88.29 kJ·mol −1 ), which led to achieve low-temperature H 2 evolution at 95 °C. Additionally, this work demonstrates the excellent photothermal stability of Cu 2 O/Ti 3 C 2 T x @TiO 2 under without KOH condition (average rate 2383.2 μmol g cat −1 h −1 in 72 h), and a total turnover number (TON) up to 1373.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Peng Li,Chao Ma,Ning Li,Chi Tang,Zhaolin Lv,Zhenjie Gu,Zhihua Qiao,Chongli Zhong
Metal-organic framework (MOF) membranes have demonstrated significant potential in replacing traditional polymer membranes for gas separation. However, synergistically enhancing gas permeance and selectivity remains challenging in MOF membrane design, particularly when framework pore apertures surpass gas kinetic diameters. Here, an innovative strategy is reported for engineering ultrathin ZIF-8 membranes with chemical adsorption sites via polymer bidirectional induction. The polyethyleneimine (PEI)-Zn 2+ interface layer facilitated the formation of ultrathin ZIF-8 membranes (~78.4 nm) by guiding small-sized crystal growth. Meanwhile, the competitive coordination of PEI with 2-methylimidazole induced the pendant of partially coordinated ligands in the ZIF-8 cavity to form chemisorption sites. This structural alteration enabled the in-situ chemical adsorption of CO 2 in the cavity of ZIF-8, thus contracting the window apertures and enhancing the molecular sieving efficiency. As a result, the ultrathin ZIF-8 membrane exhibited an excellent H 2 /CO 2 ideal selectivity of 34.2 with a remarkable H 2 permeance of 7143.6 GPU in single-gas tests, outperforming other reported ZIF-8 membranes. During mixed-gas H 2 /CO 2 testing, the in situ structural changes demonstrated robust pressure-performance stability and long-term gas separation capability. This work advances the development of ZIF-8 membranes for efficient separation of H 2 /CO 2 , and offers a feasible design principle and theoretical guidance for MOF-based gas separation membranes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Jingting Sun,Shangshang Wang,Xingyu Liu,Huan Yu,Jiaming Li,Chao Liu,Qinfang Zhang,Zhigang Zou
Photocatalytic hydrogen production (PHE) technology has emerged as a sustainable approach to convert solar energy into hydrogen energy, exhibiting significant potential for clean energy applications. In this study, an ultrasonic-assisted method was adopted to fabricate S-scheme MoSe 2 /Mn 0.5 Cd 0.5 S (MoSe 2 /MCS) composites, where intimate heterostructures are formed through interfacial Mo–S bonds between MCS and MoSe 2 . The atomic-level Mo–S bonds establish charge transport pathways and enable directional control of charge transfer. The as-constructed S-scheme MoSe 2 /MCS photocatalysts exhibit two critical advantages: enhanced charge carrier separation rate and improved overall redox capacity. Under visible-light irradiation, the MoSe 2 /MCS composites significantly outperform pure MCS in PHE performance. The optimal 5-MoSe 2 /MCS composite demonstrates the superior PHE activity, achieving an apparent quantum yield value of 71.16 % at 400 nm and remarkable photocatalytic stability. Key characterization techniques, including (solution-based) time-resolved photoluminescence technique, theoretical calculation, photoelectrochemical measurements, were employed to elucidate the positive correlation between ion-carrier interaction and charge separation efficiency, thereby enhancing the PHE performance. Based on experimental analysis and theoretical calculation, a plausible PHE mechanism for the S-scheme MCS composites is revealed and discussed in detail. These findings provide valuable insights for designing high-efficiency S-scheme heterostructured composites with interfacial chemical bonds.
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