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ACS Applied Materials & Interfaces · 2018 · IF 8.097

A GO-Induced Assembly Strategy To Repair MOF Nanosheet-Based Membrane for Efficient H2/CO2 Separation

Fangfang Yang,Mian Wu,Yuchao Wang,Saeed Ashtiani,Heqing Jiang

Metal–organic framework (MOF) nanosheets have emerged as promising materials for the construction of molecular sieve membranes due to their nanoscale thickness and highly oriented pore arrays. However, the development of defect-free MOF nanosheet membranes from rigid MOF nanosheets with efficient permselectivity and robust mechanical strength still remains a big challenge. Herein, we develop a facile GO-induced assembly strategy to design continuous and uniform two-dimensional MOF composite membranes, in which the copper 1,4-benzene dicarboxylate (CuBDC) nanosheets present a layer-stacking arrangement. With the assistance of flexible GO, the voids between the junctions of rigid MOF nanosheets are well-repaired, and the interlayer bonding interactions are strengthened, resulting in the fabrication of a continuous nanosheet membrane with robust mechanical strength. The obtained MOF nanosheet-based membranes display remarkable H2/CO2 separation performance with a superior H2 permeance of 9.6 × 10–7 mol m–2 s–1 Pa–1 and an ideal separation selectivity of 95.1 due to the well-defined size exclusion effect, showing great promise for H2 separation and purification. The repair strategy described here could also provide the blueprint for the development of other nanosheet-based membranes.

CAS / MDL: 75-05-8 100-21-0
研究领域: 材料科学 · 化学工程 · 纳米技术
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CHEMICAL ENGINEERING SCIENCE · 2025 · IF 4.3

Fabrication of defect-free MIL-96 membrane via aluminum isopropoxide gel layer towards exceptional H2/CO2 separation

Qian Yu,Bilin Liang,Siqi Jia,Fang Li,Qiming Li

A novel approach was developed to fabricate defect-free MIL-96 membranes on an α-Al 2 O 3 support by combining aluminum isopropoxide coating with mixed-solvent regulation. The aluminum isopropoxide gel on the support functions as an active Al source, directing MIL-96 crystal nucleation and growth. A subsequent secondary crystallization can produce a well-intergrown MIL-96 membrane. Here, the gel coating inhibits the preferential crystallization of MIL-96 particles in the support pores, optimizing the microstructure and diminishing inter-crystal defects. By accurately adjusting the formic acid to N-methylformamide ratio in synthesis solution, a balance between membrane crystallinity and formation is achieved. Membrane separation property evaluation revealed an outstanding H 2 permeance of 1800 GPU and an H 2 /CO 2 separation factor of over 24.0, outperforming some advanced polycrystalline MOF membranes. This approach provides a potentially cost-efficient method for the large-scale preparation of MIL-96 membranes, holding great potential for practical applications in membrane separation.

CAS / MDL: 1344-28-1 554-95-0
研究领域: 材料科学 · 化学工程
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Nano Research · 2021 ·Vol. 15 ·期 1 ·528-534 · IF 8.897

Phase and structure modulating of bimetallic Cu/In nanoparticles realizes efficient electrosynthesis of syngas with wide CO/H2 ratios

Shen Chenqi,Wang Pengtang,Li Leigang,Huang Xiaoqing,Shao Qi

Syngas (CO + H 2 ) is the incredibly important feedstock for producing synthetic fuels and various value-added chemicals. CO 2 electrochemical reduction to syngas is an environmental-friendly and sustainable approach, but still challenging to produce tunable syngas with a wide ratio of CO/H 2 . Herein, by modulating the structure and phase, we have successfully obtained a series of copper-indium (Cu-In) catalysts, which are efficient for producing syngas with tunable CO/H 2 ratios. A series of CuIn bimetallic catalysts with different structures from hollow sphere to two-layer hollow sphere and different phases from CuO to Cu 2 O are developed. We find that the CO and H 2 are the only gaseous products, in which the CO/H 2 ratios can be readily tuned from 1.2 ± 0.1 to 9.0 ± 1.5 by simply controlling the thermal annealing temperature. It also exhibits high durability during a 10-h test. The unique performance is attributed to the modulated In enrichment on the Cu surfaces during the CO 2 reduction reaction, which causes the differences in binding energies for key reaction intermediates, thus resulting in the tunable composition of syngas. The present work emphasizes a simple yet efficient phase and structure modulating strategy for designing potential electrocatalysts for producing syngas with widely tunable CO/H 2 ratios.

研究领域: 材料科学 · 能源化学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Co3O4–CuCoO2 Nanomesh: An Interface-Enhanced Substrate that Simultaneously Promotes CO Adsorption and O2 Activation in H2 Purification

Junfang Ding,Liping Li,Haorui Zheng,Ying Zuo,Xiyang Wang,Huixia Li,Shaoqing Chen,Dan Zhang,Xingliang Xu,Guangshe Li

Nanomaterials are widely used as redox-type reaction catalysts, while reactant adsorption and O2 activation are hardly to be promoted simultaneously, restricting their applications in many important catalytic fields such as preferential CO oxidation (CO-PROX) in H2-rich stream. In this work, an interface-enhanced Co3O4–CuCoO2 nanomesh was initially synthesized by a hydrothermal process using aluminum powder as a sacrificial agent. This nanomesh is systematically characterized by powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N2 adsorption, X-ray photoelectron spectroscopy, UV–vis absorption spectroscopy, Raman spectroscopy, X-ray absorption near-edge spectroscopy, hydrogen temperature-programmed reduction, and oxygen temperature-programmed desorption. It is demonstrated that the nanomesh possesses high-density nanopores, enabling a large number of CO adsorption sites exposed to the surface. Meanwhile, electron transfer from O2– to Co3+/Co2+ and the weakened bonding strength of Co–O bond at surfaces promoted the oxygen activation and redox ability of Co3O4. When tested as a catalyst for CO-PROX, this nanomesh with an optimized pore structure and a surface electronic structure, exhibits a strikingly high catalytic oxidation activity at low temperatures as well as a broader operation temperature window (i.e., CO conversion >99.0%, 100–200 °C) in the CO selective oxidation reaction. The present finding should be highly useful in promoting the quest for better CO-PROX catalysts, a hot topic for proton exchange membrane fuel cells and automotive vehicles.

CAS / MDL: 7429-90-5
研究领域: 催化材料 · 能源化学 · 燃料电池
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Improved naphthalene photodegradation rate of CN/Pt-P25 photocatalyst by effectively tuning Pt chemical states via H2 secondary annealing

Yu Huang,Xinyang Xu,Fengkun Han,Xi Chen,Guangjian Fan

Photocatalytic technology holds promising prospects for remediating naphthalene pollution in water bodies. In this work, the CN/Pt-P25 photocatalyst was successfully prepared via photodeposition combined with co-pyrolysis methods, and employed for naphthalene photodegradation under simulated sunlight. The chemical state of Pt was found to have a significant impact on the photocatalytic activity. H 2 secondary annealing effectively tuned Pt chemical states, increasing the proportion of Pt 0 species on the CN/Pt-P25 photocatalyst from 41.91 % to 62.24 %. The improved proportion of Pt 0 species proportion led to a reduction in the bandgap, which induced changes in the band positions and notably enhancing the separation efficiency of photogenerated electron-hole pairs. Under simulated sunlight irradiation, (H 2 ) CN/Pt-P25 photocatalyst achieved complete naphthalene photodegradation within 100 min. Thus, photocatalysts containing a high proportion of Pt 0 species exhibited an improved performance in naphthalene photodegradation. These findings provide new insights into the application of photocatalytic technology for the remediation of PAHs.

CAS / MDL: 18497-13-7
研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Efficient activity of CoCu@SiC catalytic ceramic membrane via H2 reduction treatment for pollutants degradation

Xing Liu,Jing Wang,Yuting Zhang,Gang Guo,Jiakuan Yang,Shushan Yuan,Bart Van der Bruggen

Catalytic ceramic membranes (CCM) have attracted increasing attention in membrane material research due to their catalytic and separation functions. However, it is difficult to obtain stable CCM with excellent catalytic performance via common methods. Herein, SiC ceramic membrane loaded with Co, Cu bimetal were prepared by vacuum filtration method and heat treated at H 2 atmosphere (CoCu@SiC-H CCM). Results confirmed that heat-treated at H 2 atmosphere can enhance the catalytic performance of membrane. The first-order rate constant of the CoCu@SiC-H CCM/ peroxymonosulfate(PMS) system reached 0.01473 ms −1 , which is 10 3 -10 5 times greater than previously researches (0.0409–0.7588 min −1 ). Optimal CoCu@SiC-H CCM/PMS system achieved 98.02 % degradation of sulfamethoxazole in 1 min. The CoCu@SiC-H CCM presents outstanding catalytic performance due to the generation of Co 0 and the increase of oxygen vacancy concentration. OH and SO 4 − play important roles in the CoCu@SiC-H CCM/PMS degradation system. This work provides a new design method for preparing catalytic ceramic membranes with excellent catalytic performance, which can efficiently treat refractory wastewater in harsh environments.

研究领域: 环境科学 · 材料科学
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Surfaces and Interfaces · 2025 · IF 6.3

Enhanced C-C coupling selectivity by sulfur vacancy for photocatalytic pyridinemethanol conversion with simultaneous H2 evolution

Ting Li,Jiantao Bi,Huajing Li,Qing Li,Yuangang Li

The synergistic coupling of photocatalytic C C bond construction and H 2 evolution presents a promising strategy for concurrent organic synthesis and sustainable H 2 evolution. Nevertheless, precisely regulating the reaction pathways to enhance the selectivity of target products remains a challenging. Here, the Sv-CdS/TiO 2 Ni 2 P photocatalyst containing sulfur vacancies was synthesized via calcination, achieving highly selective conversion of 4-pyridinemethanol into the C C coupling product 1,2-di-(4-pyridyl)-1,2-ethanediol under visible-light irradiation, with a selectivity of 96.59 %. In comparison, the M-CdS/TiO 2 Ni 2 P photocatalyst prepared by mechanical mixing exhibits superior H 2 evolution activity of 6.48 mmol·g -1 ·h -1 . Mechanism studies reveal that 4-pyridinemethanol interacts with the Sv-CdS/TiO 2 Ni 2 P photocatalyst through the N atom, which preferentially activates the sp 3 C H bond of 4-pyridinemethanol to generate •CH(OH)C 5 H 4 N radical for further C C coupling reaction. This work not only highlights the selective regulation of the 4-pyridinemethanol C C coupling pathway by sulfur vacancies engineering, but also provides new insights for achieving efficient photocatalytic organic synthesis and green H 2 evolution.

CAS / MDL: 10022-68-1 7791-20-0
研究领域: 光催化 · 有机合成 · 材料科学 · 环境化学 · 能量转换
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Green Energy & Environment · 2020 · IF 6.395

Engineering three-layer core–shell S-1/TS-1@dendritic-SiO2 supported Au catalysts towards improved performance for propene epoxidation with H2 and O2

Zhaoning Song,Juncong Yuan,Zhenping Cai,Dong Lin,Xiang Feng,Nan Sheng,Yibin Liu,Xiaobo Chen,Xin Jin,De Chen,Chaohe Yang

The advocacy of green chemical industry has led to the development of highly efficient catalysts for direct gas-phase propene epoxidation with green, sustainable and simple essence. The S-1/TS-1@dendritic-SiO 2 material with three-layer core–shell structure was developed and used as the support for Au catalysts, which showed simultaneously fantastic PO formation rate, PO selectivity and stability (over 100 h) for propene epoxidation with H 2 and O 2 . It is found that silicalite-1 (S-1) core and the middle thin layer of TS-1 offer great mass transfer ability, which could be responsible for the excellent stability. The designed dendritic SiO 2 shell covers part of the acid sites on the external surface of TS-1, inhibiting the side reactions and improving the PO selectivity. Furthermore, three kinds of SiO 2 shell morphologies (i.e., dendritic, net, mesoporous shell) were designed, and relationship between shell morphology and catalytic performance was elucidated. The results in this paper harbour tremendous guiding significance for the design of highly efficient epoxidation catalysts.

研究领域: 化学工程 · 催化材料科学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Highly Efficient Recovery of H2 from Industrial Waste by Sunlight-Driven Photoelectrocatalysis over a ZnS/Bi2S3/ZnO Photoelectrode

Yan Lu,Radian Popescu,Dagmar Gerthsen,Yichen Feng,Wei-Ren Su,Yu-Kuei Hsu,Ying-Chu Chen

Hydrogen (H2) fuel production from hazardous contaminants is not only of economic importance but also of significance for the environment and health. Hydrogen production is exemplified in this work by using bismuth sulfide (Bi2S3) sandwiched in between zinc sulfide (ZnS) and zinc oxide (ZnO) as dual-heterojunction photoelectrode to photoelectrochemically extract H2 from sulfide- and sulfite-containing wastewater, which is emitted in enormous quantities from the petrochemical industries. The H2 evolution rate over the ZnS/Bi2S3/ZnO photoelectrode under solar illumination amounts to 112.8 μmol cm–2 h–1, of which the photocurrent density in the meantime reaches 10.7 mA cm–2, by far exceeding those reported for additional Bi2S3-based counterparts in the literature. Such superior performance is ascribed on one hand to the broadband sunlight-harvesting ability of Bi2S3 that gives rise to respectable photoexcited electron–hole pairs. These photogenerated charge carriers are subsequently rectified by the built-in electric field at the ZnS/Bi2S3 and Bi2S3/ZnO heterojunctions to flow in the opposite directions to well circumvent the recombination losses and, most importantly, in turn contribute substantially to the H2 evolution reaction.

研究领域: 环境科学 · 化学工程 · 材料科学 · 可再生能源
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ChemistrySelect · 2024 ·Vol. 9 ·期 32 ·e202402012 · IF 1.9

Impact of H2 Reduction on the Performance and Stability of Phenol Catalytic Wet Air Oxidation (CWAO) Over Cu−Ce/AC Catalysts

KangDi Chen,Siqi Chai,Guoqiang Li,Zeyu Li,Youqian Wang,Heting Li,Liwei Ma,Mai Wei,Guojie Zhang,Ying Wang

Graphical H 2 reduction reduces part of Cu 2+ to Cu + and Ce 4+ to Ce 3+ on the catalyst surface, and Cu and Ce can be stably anchored on the surface of the Cu−Ce/AC catalyst, which effectively improves the dispersion of the Cu component, and then slows down the loss of metal Cu. In this study, we utilized the carbon precursor derived from walnut shells to synthesize a series of Ce-modified Cu-based carbon catalysts (Cu−Ce/AC) via the impregnation method. We investigated the performance and stability of Cu−Ce/AC catalysts for CWAO phenol after H 2 reduction at various temperatures. The Cu−Ce/AC-250 catalyst exhibited its highest performance at 250 °C, achieving complete phenol conversion. Characterization results from techniques including XRD, BET, FTIR, ICP-OES, SEM-EDS, XPS, and H 2 -TPR indicated that the active components of the H 2 -reduced catalysts were more evenly distributed across the catalyst surface, thereby enhancing the availability of reactive sites for phenol oxidation. Simultaneously, under the appropriate temperature, the H 2 atmosphere can reduce a portion of the Cu 2+ on the catalyst surface to Cu + , thereby mitigating the loss of Cu components.

研究领域: 环境科学 · 催化化学
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Applied Food Research · 2025 · IF 6.2

Development of a Captiva EMR-lipid clean-up and LC-MS/MS methodology for detecting H2 receptor antagonists in functional foods and food-medicine homology materials

Guodong Shan,Xiuqin Fan,Qingcheng Wang,Li Zhang,Lijun Ge,Weibo Lu,Jing Xue,Kang Chen,Zejun Wang,Qing Shen

The inappropriate use of H2 receptor antagonists (H2RAs) in functional foods (FFs) and food-medicine homology materials (FMHs) designed to enhance gastrointestinal function (IGF) presents health risks due to potential adverse effects. In this study, an analytical method that integrates Captiva EMR-Lipid (CEL) solid-phase extraction (SPE) with liquid chromatography tandem mass spectrometry (LC-MS/MS) has been developed for the detection of H2RAs (nizatidine, famotidine, cimetidine, ranitidine, and lafutidine) in these products. Through the optimization of CEL-SPE parameters, such as using 200 mg of sorbent and eluting with ACN/water (80/20, v/v), the recovery rates of H2RAs in IGF-FF and IGF-FMH ranged from 87.4 % to 94.6 % and 90.2 % to 97.1 %, respectively. The assessment of matrix effects revealed that the five H2RAs exhibit matrix suppression, necessitating the construction of matrix-matched standard curves with correlation coefficients (r 2 ) exceeding 0.9991. The detection limits ranged from 0.4 to 0.8 μg·kg −1 and the quantification limits ranged from 1.3 to 2.7 μg·kg −1 , with recovery rates spanning from 85.4 % to 97.1 % and relative standard deviations ≤ 15 %. The successful development of this technique not only helps safeguard consumer health but also provides scientific basis and technical support for market supervision, thereby preventing and addressing food safety risks.

研究领域: 食品安全 · 分析化学 · 药物检测
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ACS Applied Energy Materials · 2022 · IF 6.959

Effectively Tuning the Ratio of CO and H2 into Syngas through CO2 Electrochemical Reduction over a Wide Potential Range on a ZnO Nanosheet via Ni Doping

Jiale Wang,Qian Xiang,Wencong Zhang,Fenglei Shi,Fan Li,Peng Tao,Chengyi Song,Wen Shang,Tao Deng,Jianbo Wu

Electrochemical CO2 reduction (ECR) into syngas is a promising method to reduce CO2 in the atmosphere. However, balancing the activity of ECR and hydrogen evolution reaction (HER) and controlling the stable CO/H2 ratios in a large potential range for the industrial desired syngas are still challenging. Herein, a low-cost Ni-doped ZnO nanosheet array on a zinc foil is synthesized via a convenient hydrothermal method to produce a controllable ratio of CO/H2 into syngas. Because of the lower impedance and larger electrochemical area, Ni-doped ZnO has a more significant current density. Furthermore, by adjusting the Ni doping content in the ZnO nanosheet, the activity of ECR and HER could be controlled, and the ratio of CO/H2 can be tuned from 0.1 to 4.5 over a wide potential range (−1.2 to −1.8 V vs reversible hydrogen electrode, RHE), surpassing most of the reported work. Such a wide range and stable ratio of CO/H2 in a broad potential range makes it possible to convert CO2 into feedstock for many essential chemical products.

研究领域: 材料科学 · 环境科学
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