Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Wanpeng Zhou,Ruyao Feng,Miaolian Ma,Zhixuan Hu,Tao Yao,Maofeng Zhang
Natural flavonoids, including quercetin, rutin, baicalein and puerarin have been employed for the first time as efficient catalysts in the alcoholysis of NaBH 4 . Among them, quercetin demonstrates optimal catalytic performance for this reaction, achieving an HGR value of 26374 mL H 2 g cat −1 min −1 when 0.2 g NaBH 4 is catalyzed by 50 mg quercetin. The catalytic activity of quercetin is unparalleled for methanolysis of NaBH 4 , particularly at low-temperature; notably, a high HGR value of 1948 mL H 2 g cat −1 min −1 is observed even at −25 °C. Furthermore, the activation energy for the NaBH 4 methanolysis catalyzed by quercetin within a low temperature range of −25 to 25 °C has been calculated to be 17.2 kJ mol −1 . Investigates into the reusability and regeneration of quercetin reveal that over 74 % of its catalytic activity is retained after five consecutive uses; additionally, complete recovery of catalytic activity can be achieved through simple acid treatment. Moreover, kinetic studies indicate that the reaction orders of NaBH 4 methanolysis catalyzed by quercetin obey to first-order kinetics concerning all concentrations: NaBH 4 concentration, catalyst dosage, and methanol content. This study establishes a foundation for practical application involving NaBH 4 in hydrogen production under cold climate conditions typical in Polar Regions or during severe winters at northern latitudes.
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高影响因子
APPLIED ENERGY
·
2024
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IF 10.1
Jiecheng Zou,Lanxun Zhao,Qiang Hu,Dingding Yao,Haiping Yang
The gasification technology has shown great potential to upcycle plastic waste for clean and high-value fuel. Gasification of disposable plastic masks was investigated in a two-stage pyrolysis-catalytic reforming system, aiming at producing the syngas with flexible H 2 to CO ratio which can be tuned for various downstream applications without further purification and adjustment. To maximize the syngas yield and minimize the carbon deposition, different gasifying agents in the staged catalytic process was explored. The results showed that CO 2 significantly promoted syngas production mainly by increasing CO yield. However, H 2 -rich syngas was obtained via using steam as the gasifying agent. Competitive and synergistic relationships between CO 2 and H 2 O agent at co-feeding process were further revealed. CO 2 facilitated the reforming of H 2 O at low dose of steam while exhibiting a main competition with adequate steam except for synergy at 5 mL/min CO 2 flow rate. An optimum H 2 -rich syngas yield of 135.59 mmol/g plastic with H 2 /CO ratio of 2 was obtained at co-feeding reactants. Therefore, the co-feeding of H 2 O and CO 2 could show positive effect for both coke removal and syngas quality regulation. Results found in this work increased the overall operational flexibility and economy of pyrolysis and catalytic reforming of plastic waste.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Zhengjiang Liu,Dan Zhou,Huiyan Ma,Lei Xing,Qiancheng Zhang,Juming Liu
SO 4 2− /CeO 2 /TiO 2 composite oxides are successfully fabricated via sol-gel method and impregnation process for photocatalytic H 2 production. The characterization results from XRD, FTIR and TEM revealed that the heterojunctions were formed by the formation of Ti-O-Ce bond across the SO 4 2− /CeO 2 /TiO 2 interface, which was contributed significantly to separation of photo-generated carriers. Py-FTIR spectra and XPS results indicated that Lewis acid and Brønsted acid sites were formed over the surface of SO 4 2− /CeO 2 /TiO 2 composite, which was owing to SO 4 2− coordinated to the metal on the sample surface. The induced Lewis acid sites could enhance the separation of photogenerated carriers, and Brønsted acid sites could provide protons for photocatalytic H 2 production. In addition, the Lewis acidity could facilitate the shift of conduction band minimum to a more negative value, which improves the photocatalytic H 2 production capacity of SO 4 2− /CeO 2 /TiO 2 . The results of photocatalytic H 2 production revealed that SO 4 2− /CeO 2 /TiO 2 composite exhibits superior photocatalytic activity compared to bare CeO 2 , TiO 2 and CeO 2 -TiO 2 composite. Notably, it achieves the average H 2 yield rate of 6295.2 μmol· g −1 h −1 over a period of 5 h. Combine the results of spectra analysis and photocatalytic activity H 2 evolution, it can be concluded that the synergetic effects of heterojunction structure of CeO 2 /TiO 2 composite and acid impregnation promoted the photocatalyst activity.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Ying Wu,Wenhui Fang,Min Li,Yutao Cao,Wei Cui,Zengxi Li,Hong Zhao
Electrochemical upgrading of biomass waste (such as glycerol)-assisted water electrolysis for the production of valuable formate and high-purity hydrogen offers a promising route to develop sustainable and clean sources of energy. Herein, using a simple two-step electrodeposition method to implant CuNi alloy in VOx-doped Ni (NiVOx), we construct a competent, stable, and bifunctional heterogeneous catalyst (CuNi–NiVOx) toward hydrogen evolution reaction (HER) and glycerol electrooxidation reaction (GER). The CuNi–NiVOx electrode presents excellent HER activity with an ultralow overpotential of 8 mV in 1.0 M KOH to deliver a current density of 10 mA cm–2 and high GER activity for selective formate production with high Faradaic efficiency (FE). Moreover, the hybrid electrolytic cell formed by the bifunctional CuNi–NiVOx catalyst was able to reach a current density of 10 mA cm–2 with an ultralow voltage (1.308 V). X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations confirm the existence of electron transfer between the O sites and metal sites and between heterogeneous interfaces, thus optimizing the hydrogen adsorption ability (0.02 eV). This work may provide ideas for the engineering of heterogeneous dual-function electrocatalysts for energy-saving hydrogen production and simultaneous highly selective production of formate.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Xiaoman He,Zhangdi Peng,Peilin Shen,Chenjia Miao,Jiale Xie,Chen Deng,Panagiotis G. Kougias,Dekui Shen,Richen Lin
Conversion of CO2 and H2 into biomethane is a promising technology within the concept of power-to-X. However, the integration of high-value-added products can enhance the economic viability and diversify future biobased production chains. Herein, an integrated biosystem converting CO2/H2 into acetic acid, which is further converted to C4+ fatty acids, was demonstrated with the aim to assess the role of carbonaceous materials (model nanomaterial graphene and cost-effective biochar) and external electron donor (ethanol). With the supplementation of ethanol as the electron donor, carbonaceous materials significantly increased the production and selectivity of butyrate (C4) and caproate (C6) due to enhanced microbial growth and chain elongation efficiency. The highest concentration of butyrate (2512.35 ± 60.05 mg/L) was observed in the graphene-added group, while the highest concentration of caproate (396.74 ± 14.83 mg/L) was observed in the biochar group, suggesting different mechanisms induced by carbonaceous materials. Microbial community analysis revealed that carbonaceous materials primarily enriched members of the genus Clostridium_sensu_stricto_12, which are identified as typical carbon chain elongating microorganisms. Functional prediction revealed that carbonaceous materials increased the relative abundance of functional genes encoding crucial enzymes involved in both the Wood–Ljungdahl pathway and the fatty acid biosynthesis pathway. This study demonstrated an integrated approach for the efficient conversion of CO2 to value-added green chemicals.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2025
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IF 4.7
Jingbiao Ge,Huihui Xue,Yang Yang,Sujuan Zhang,Xiuzhen Zheng,Shifu Chen
To optimize the performance of photocatalytic H 2 production, various effective strategies have been developed to design highly efficient photocatalysts, including morphology control, synergistic reaction design, and utilization of photogenerated charge carriers (PCCs). In this study, a highly efficient Bi-Bi 2 WO 6 /Zn 0.5 Cd 0.5 S (BBWO/ZCS) composite was synthesized by embedding Zn 0.5 Cd 0.5 S (ZCS) nanospheres into Bi-Bi 2 WO 6 (BBWO) microsheets through electrostatic self-assembly method. Although BBWO show poor activity in H 2 generation, it largely improves the performance of ZCS under visible light illumination. When the mass of BBWO is 3 % in the composite, BBWO/ZCS exhibited the highest H 2 production rate (28.0 mmol g −1 h −1 ), much higher than that of pure ZCS. Meanwhile, its apparent quantum efficiency (AQE) is high to 8.45 % at 400 nm. The design of the BBWO/ZCS composite not only improves the migration and utilization efficiency of PCCs, but also offers valuable theoretical insights and experimental references for the development of highly efficient photocatalysts.
研究领域:
材料科学
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光催化
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可再生能源
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纳米材料
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环境科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Qian Wu,Xinping He,Chenyi Cui,Chenchen Jiao,Baojin Qi,Jinjia Wei
Mixed matrix membranes (MMMs) incorporating metal–organic frameworks (MOFs) hold significant promise for gas separation applications. However, the inherent disparity between the organic polymer matrix and the inorganic fillers frequently leads to interfacial incompatibility issues. In this study, we adopted an in-situ interfacial crosslinking strategy to fabricate MMMs incorporating NH 2 -Zn 2 (Bim) 4 nanosheets that simultaneously act as nanofillers and reactive crosslinkers. Specifically, during the thermal imidization reaction process, the amino groups of NH 2 -Zn 2 (Bim) 4 not only establish hydrogen bonding interactions with the carbonyl groups of polyamic acid (PAA) (the precursor of polyimide), but undergo dehydration reactions with carboxyl groups, leading to the formation of stable amide linkages. Meanwhile, the aromatic structure of the BI units, a key monomer of polyimide, closely resembles that of the ligands of NH 2 -Zn 2 (Bim) 4 , which can establish π-π stacking interactions, further improving the interfacial compatibility between the polymer matrix and MOF fillers. Among the prepared samples, MMMs incorporating 33.3 wt% NH 2 -Zn 2 (Bim) 4 nanosheets exhibit the maximum H 2 permeability of 680.5 Barrer, and its H 2 /N 2 and H 2 /CO 2 selectivities were 18.7 and 13.3, respectively, which were close to or even exceeded the Robeson upper bound. The proposed in-situ interfacial engineering based on chemical crosslinking provides a novel and effective route for fabricating high-performance MMMs with enhanced interfacial compatibility, demonstrating great potential for hydrogen separation applications.
研究领域:
材料科学
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膜技术
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气体分离
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化学工程
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纳米复合材料
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高影响因子
JOURNAL OF CATALYSIS
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2023
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IF 7.3
Da Yang,Cong-Kun Zhong,Lu-Yao Tian,Long-Li Zhang,Huan Liu
Formic acid (FA) is a potential hydrogen storage substance due to its abundant resources, ease of storage, and high hydrogen content. In this paper, the hydroaminomethylation of olefins with FA as the hydrogen source was accomplished over DPEPhos-based Ru catalyst for the first time. Under optimal conditions, α-olefins or cycloolefins with steric hindrance obtained 62%∼96% yields of the target amines. The influence of FA was investigated by in situ high-pressure 1 H NMR spectroscopy analyses, isotope labelling experiments, and the separated hydroformylation or reduction amination. It was indicated that FA was decomposed to provide H 2 for the hydroformylation, and was used as a reducing agent in the transfer hydrogenation of imines/enamines. The reversible amidation of FA with substrate amine could inhibit the side reaction of aldehydes transfer hydrogenation. Moreover, the involving FA would facilitate the formation of Ru-H species, thereby promoting the hydroaminomethylation.
研究领域:
化学
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催化科学
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Yongliang Xu,Lei Xiang,Lanyun Wang,Zecheng lv,Yao Li,Hao Shao,Haidong Chen,Kun Zhang,Xiaodong Feng
Hydrate-based hydrogen storage technology enables the solid-state stabilization of hydrogen by encapsulating H 2 molecules within a clathrate lattice structure, representing a promising strategy for industrial-scale gas storage. This study focuses on enhancing the gas storage performance and stability of H 2 –CH 4 binary hydrate. Experiments on the formation and dissociation of H 2 –CH 4 hydrates were conducted under a pressure of 6.0 MPa. The study examines the effects of C 8 F 18 (6 wt%, 8 wt%, 10 wt%) and 1,3-DIOX (4mol%, 5mol%, 6mol%) on H 2 –CH 4 (with a ratio of 1:1) hydrate. The results indicate that in the composite systems containing 5mol%, 1,3-DIOX and 8 wt% C 8 F 18 , a synergistic promotion effect was observed. The nucleation temperature was further increased by 3.8 K compared to the single 1,3-DIOX system. The induction time was shortened by 146.9 min. Gas consumption improved to 0.14446 mol. Furthermore, In 4mol%1,3-DIOX and 6 wt% C 8 F 18 compound system prolonged the pre-dissociation 48.33min relative to the 1,3-DIOX system. C 8 F 18 enhances the self-preservation of the hydrate, an effect that is not present with only 1,3-DIOX. This effect becomes more pronounced as the concentration of C 8 F 18 increases. Generally, the 1,3-DIOX + C 8 F 18 can play a synergistic effect on enhancing the gas storage performance and stability of hydrates.
研究领域:
物理化学
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能源材料
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气体储存
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水合物化学
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工业催化
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高影响因子
NANOTECHNOLOGY
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2019
·Vol. 31
·期 9
·095406
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IF 3.399
Weisheng Lei,Fengzhi Wang,Xinhua Pan,Bin Lu,Zhizhen Ye
Plasmonic noble metal has been applied in photocatalytic materials, and TiO2 with plasmonic noble metal has been studied for a long time. In this work, we have fabricated incomplete covered Au/Ag alloy nanoshuttle-TiO2 nanomaterials with 268.7 μmol g−1 h−1 H2-evolution in a simple solution method. The considerable photocatalytic performance is mainly due to the enhanced surface plasmon resonance effect of Au/Ag alloy nanoshuttles. It has been found that TiO2 clusters attached to the Au/Ag nanoshuttles surface migrate under electrons irradiation and cover the exposed Au/Ag NS surface to achieve thermodynamic stability, which results in instability of photocatalytic performance. The mechanism has been discussed in detail.
研究领域:
材料科学
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纳米技术
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能源科学
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高影响因子
Journal of Nanomaterials
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2022
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IF 3.791
Haomiao Tang,Wenbin Wang,Jun Zhou,Tiantian Li,Zhu Shu
Polymeric carbon nitride (PCN), as a metal-free photocatalyst, has drawn wide attention in the photocatalytic H2 evolution. However, the photocatalytic activity of directly synthesized PCN is limited by its low crystallinity. Currently, regulating the melon-based PCN into tri-s-triazine-based crystalline PCN to further optimize its structure has been proved to effectively improve its photocatalytic activity. The heptazine-based crystalline carbon nitride, potassium poly(heptazine imide) (abbreviated as K-PHI), has been used in photocatalytic H2 evolution benefiting from its high crystallinity, as the high crystallinity narrows the bandgap and increases the light capture efficiency and increases the charge mobility. Nevertheless, the effect of synthesis temperature on crystallinity has not yet been reported. In this work, the effect of temperature on the crystallinity of heptazine-based crystalline carbon nitride was studied by one-step synthesis at different temperatures. It shows that the heptazine-based crystalline structure appears when the temperature exceeds 540°C. Additionally, the crystallinity of all samples is gradually improved with increasing temperature until the sample begins to decompose beyond 630°C. The sample synthesized at 630°C demonstrates the highest photocatalytic H2 evolution rate of 1.798 mmol h−1 g−1 under visible light irradiation, which is 31.5 times that of bulk PCN. Based on systematic material characterizations, the mechanism of the effect of synthesis temperature on crystallinity and the contribution of crystallinity to photocatalytic efficiency were revealed.
研究领域:
材料科学
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能源化学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Jiamin Huang,Guanghui Zhang,Jie Zhu,Mingrui Wang,Fanshu Ding,Chunshan Song,Xinwen Guo
The catalytic conversion of CO2 to higher alcohols (HAs, representing ethanol and alcohols with more than two carbon atoms) has been of great interest to mitigating the greenhouse effect and effectively utilizing CO2. However, most present catalysts have disadvantages of poor activity (conversion less than 30%) and selectivity (less than 10%) and high price. Herein, we report a Mn- and K-modified iron carbide catalyst that offers a CO2 conversion higher than 40% and a selectivity of higher alcohols exceeding 10%, and the proportion of propanol and butanol in alcohol products is more than 30%. Unpromoted iron carbide has a strong ability of hydrocarbon chain growth, leading to the fast formation of hydrocarbon products rather than HAs. However, on the Mn- and K-modified iron carbide catalyst, K is used to increase the surface C/H ratio of the catalyst by enhancing the adsorption of CO2 on the catalytic surface. The increased C/H ratio is indispensable to the formation of HAs, and the addition of Mn promoter dramatically improves the production of HAs, especially the formation of propanol and butanol. The synergistic effect between Mn and K on iron carbide is the key to produce HAs. In addition, the Mn- and K-modified iron carbide is of low cost, which can potentially provide an alternative for the hydrogenation of CO2 to produce valuable chemicals.
研究领域:
催化化学
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环境科学
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能源科学
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高影响因子
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