Journal of Materials Chemistry A
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2025
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IF 9.5
Ashfaq Ahamd,Chaoran Zhang,Yichuan Gu,Qu Jiang,Ziyang Sheng,Ruohan Feng,Sihong Wang,Haoyue Zhang,Qianqing Xu,Zijian Yuan,Fang Song
Ordered mesoporous materials offer significant advantages in reducing energy barriers, tuning intrinsic reaction pathways, and suppressing undesirable side reactions in electrocatalytic CO2 reduction reactions (CO2RR). Here, we present a straightforward method for the direct electrodeposition of ordered mesoporous CO2RR catalysts on a carbon-based porous transport layer, utilizing lyotropic liquid crystals (LLCs) as templates. The versatility of this method was demonstrated with tin-, bismuth-, and indium-based catalysts, all exhibiting pore sizes on the order of several nanometers. These ordered mesoporous catalysts efficiently and selectively drive CO2RR toward the value-added product of formate. They achieve partial current densities that are 3 to 8 times higher than those of disordered mesoporous reference samples, with a faradaic efficiency (FE) of up to 93% at an optimal potential of −0.9 V vs. RHE. In a flow cell configuration, Sn-based catalysts deliver a current density of ∼200 mA cm−2 over 22 hours at a potential of only −0.65 V vs. RHE. Spectroscopic and electrochemical analyses suggest that the high performance can be attributed to the exclusive exposure of active sites for the formate, improved mass transport, and modulated local microenvironments. Our work demonstrates a simple yet effective method for the direct deposition of efficient and selective catalysts onto electrodes. The insights gained from the underlying mechanisms provide valuable guidance for the design of high-performance CO2RR electrocatalysts.
研究领域:
材料科学
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电化学
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催化科学
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DOI
高影响因子
Recycling
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2025
·Vol. 10
·期 1
·10
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IF 4.6
Xin Hong,Jingyi Chen,Jing Wei,Wenjie Wu,Ziyan Yang,Jing Chen,Shuchen Sun,Faxin Xiao,Ganfeng Tu
As environmental awareness grows, hydrodesulfurization (HDS) catalysts have become crucial in petroleum refining, yet their use results in oil-laden waste, poses environmental risks, and complicates subsequent treatment. Efficient oil removal is thus critical for processing spent catalysts. This study systematically compares three de-oiling methods, extraction, chemical thermal washing, and pyrolysis, to identify the optimal de-oiling method. In the experiments, extraction achieves a 94.12% oil removal rate at a liquid-to-solid ratio of 10 mL/g, a temperature of 45 °C, and a time of 60 min, maintaining around 90% efficiency after five cycles of solvent recovery. Chemical thermal washing achieves an oil removal rate of 96.26% after 4 h at 90 °C, with 0.15 wt.% SDS, 3.0 wt.% NaOH, and a liquid-to-solid ratio of 10 mL/g. The heavy oil emulsion is then decomposed with 4% CuO and 5% H2O2. The pyrolysis method removes 96.19% of oil at 600 °C in 60 min. While the extraction and chemical thermal washing methods are effective, they produce wastewater, raising environmental concerns. In contrast, the pyrolysis method is more environmentally friendly. SEM, EDS, and FT-IR analyses show that after oil removal, the metal structures on the alumina support of the spent HDS catalyst are clearly exposed, facilitating the subsequent recovery of valuable metals.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
ACS Catalysis
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2024
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IF 11.3
Lin Zhang,Junjie Su,Chang Liu,Su Liu,Haibo Zhou,Wenqian Jiao,Yongfeng Hu,Feng Xiong,Yiqing Lu,Yingchun Ye,Xusheng Zheng,Yida Zhang,Yangdong Wang,Heyong He
Direct synthesis of aromatics from syngas (STA) over an oxide–zeolite bifunctional catalyst is promising as a petroleum alternative route. Aromatics space-time yield (STY) is a key parameter for measuring the production capacity in an industrial process. However, it is still a great challenge to achieve high aromatics STY for industrial applications. Herein, we synthesized a series of CeMnOx catalysts with a self-cleaning effect. The structures and reduction process of CeMnOx catalysts were thoroughly characterized by X-ray absorption fine structure and in situ X-ray diffraction. Changes in surface carbon species during the reaction are revealed by in situ X-ray photoelectron spectroscopy and in situ Raman spectroscopy. Our results demonstrate that the intermediates can be converted to long-chain hydrocarbon or even graphite carbon species which can cover the surface of MnOx, inhibiting the reactants from further interacting with the active sites. Ce promotion in MnOx may remove the dissociated carbon species from the oxide surface by converting excess surface carbon species into short-chain hydrocarbons; thus, the growth of graphite carbon species is inhibited. This self-cleaning effect of CeMnOx catalysts facilitates the syngas conversion via maintaining a high exposure of active sites during the reaction, especially under high pressure and temperature. The aromatics STY (on carbon base) can reach as high as 4.27 mmol g–1 h–1 over CeMnOx+HZSM-5 bifunctional catalyst, which outperforms the data previously reported.
研究领域:
催化化学
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材料科学
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能源化工
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Xiaodi Jiang,Yaoning Bai,Xu Wang,Weiyao Wang,Yuxian Duan,Yingnan Liu,Xinru Li,Zichen Wang,Jinming Cai,Xiaoming Cai,Honglin Tan
Bimetallic nanostructures are currently a hot pot material among many hydrogen generation co-catalysts. In this study, CuCo bimetallic nanostructures were formed by introducing Co into Cu as the co-catalyst for TiO 2 . Characterization results from XRD , XPS , and TEM indicated the successful preparation of the high-crystallinity, impurity-free CuCo/TiO 2 photocatalyst , with CuCo bimetallic nanoparticles uniformly dispersed on TiO 2 . After the addition of Co, density functional theory (DFT) calculations showed that the free energy of H adsorption on the Cu site was optimized from 0.27 eV to −0.56 eV, which was beneficial for hydrogen production from TiO 2 . Electrochemical characterization, photoluminescence (PL) spectroscopy, infrared (IR) thermography, and finite difference in time domain (FDTD) results showed that the bimetallic CuCo acted as the co-catalyst, which increased the temperature of the reaction system, facilitated the separation of light-generated electron-hole pairs, and accelerated the charge transfer, thus promoting the photocatalytic hydrogen generation. The findings of the photocatalytic performance demonstrate that the photocatalyst exhibits the H 2 generation rate of 1933.8 μmol/g/h, which is approximately 9 times greater than that of pure TiO 2 (213.4 μmol/g/h), when the bimetallic CuCo is loaded in the molar ratio of 5:5 and at the loading amount of 2 wt%. Additionally, the photocatalyst demonstrated excellent catalytic stability, reaching 87.1% of the initial after 16 h of cycling tests. It is foreseen that further study and optimization of various metal couplings may enable the larger widespread application of bimetals as co-catalysts for hydrogen generation.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Minmin Wang,Li Zhou,Zukun Li,Hao Xu,Yanfeng Tang
Developing highly active, highly stable, and cheap electrocatalysts for water splitting is of great significance for hydrogen production. Herein, we report an amorphous Ni(OH)2-clothed transition Ni8P3 catalyst, in which the amorphous Ni(OH)2 shell provides catalytic active sites and serves as a proton conductive encapsulation layer to ensure efficient proton supply to the active Ni8P3 sites. As expected, the Ni8P3@Ni(OH)2 catalyst exhibits significant water decomposition performance at low and high current densities of 10, 100, and 1000 mA cm–2 at 1.45, 1.71, and 2.21 V, respectively, which is comparable to those of commercial electrocatalysts. In particular, the prepared Ni8P3@Ni(OH)2 electrodes possess exceptional long-term durability (200 h) at high current (over 1 A). The significantly improved water-splitting activity and durability in alkaline medium are expected to make them attractive catalyst materials to produce renewable chemical fuels.
研究领域:
材料科学
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能源化学
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DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2019
·Vol. 95
·期 3
·798-805
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IF 2.659
Dan Luo,Shengnan Liu,Wang Yin,Shuqian Xia
BACKGROUND Fast pyrolysis of lignocellulosics has provided an abundant sugar source for production of value-added chemicals, and levoglucosan is the most representative sugar in pyrolysis liquid (bio oil). This paper explored the potential for producing methyl lactate from levoglucosan by employing the mixed catalysts of zeolite tin beta (Sn-Beta) and zeolite hydrogen beta (H-Beta). RESULTS Under the optimal conditions (at 200 °C and mixed catalysts with H-Beta:Sn-Beta ratio of 1:5), the yield of methyl lactate obtained from levoglucosan conversion was as high as 35%. And the yield was comparable to that of methyl lactate obtained from glucose conversion under the similar conditions (at 200 °C and pure Sn-Beta). In order to investigate the reason, a contrasting experiment with glucose as substrate also was carried out with the mixed catalysts. The results indicated that during the levoglucosan conversion process, ‘the methanolysis of levoglucosan’ was likely to compete with ‘the dehydration of glucose’ for the Brønsted acid sites of H-Beta. In addition, the catalytic functions of H-Beta and Sn-Beta, and the reaction pathway were deeply investigated through tracking and comparing the conversion of levoglucosan over mixed H-Beta/Sn-Beta and over pure Sn-Beta catalysts, respectively. CONCLUSION The appropriately lower ratio of H-Beta:Sn-Beta and relatively higher temperature were favorable for the reaction. H-Beta containing Brønsted acid could remarkably accelerate the conversion of levoglucosan and methyl-glucosides to glucose. Sn-Beta containing Lewis acid mainly promoted the retro-aldol condensation of glucose and formation of methyl lactate. © 2019 Society of Chemical Industry
研究领域:
化学工程
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生物质能
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催化化学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Qichao Lu,Jie Li,Chen Liang,Lei Liu,Jinxiang Dong
Under the dual pressures of oil depletion and low-carbon transition, Fischer-Tropsch synthesis (FTS) technology offers a viable option for producing high value-added lower (C 2 -C 4 ) hydrocarbons from non-oil sources. However, conventional Fe-based catalysts often suffer from deactivation due to carbon deposition and sintering. Here, we report a unique Fe-ZSM-5 catalyst synthesized by doping Fe into ZSM-5, which demonstrates excellent FTS catalytic performance. During high-temperature template removal, Fe species migrated from the zeolite framework to form highly dispersed FeO x clusters (∼2 nm). Upon treatment by syngas, these FeO x clusters aggregate to form uniformly small-sized Fe 5 C 2 @C core-shell particles distributed on ZSM-5 support. The confinement effect of the inter-crystalline structure effectively prevents the sintering of Fe 5 C 2 . The smaller Fe 5 C 2 particles exhibit controlled CO dissociation, reducing the concentration of activated carbon species (C*), and the carbon shells (∼6.5 nm) limit the departure of C*, effectively suppressing carbon deposition. This unique structure enables stable catalytic activity for over 100 hours with maintained product selectivity. The Fe-ZSM-5 catalyst achieved a C 2 -C 4 hydrocarbons selectivity of 54.52 %, nearing the 56 % theoretical limit of the Anderson-Schulz-Flory (ASF) distribution. Additionally, the hydrophobic carbon shell prevents excessive oxidation of Fe 5 C 2 , reducing CO 2 selectivity by ∼56 % compared to conventional Fe/ZSM-5 catalysts, significantly enhancing atomic utilization efficiency and aligning with the principles of green development.
研究领域:
化学工程
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材料科学
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能源催化
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DOI
高影响因子
Catalysts
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2022
·Vol. 12
·期 12
·1515
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IF 4.501
Ding Zhang,Yun-Fei Li,Li-Xue Liu,Lei Duan,Zhi-Li Ren,Shou-Dong Xu,Liang Chen,Hui-Juan Guo,Yi Huang,Li-Juan Shi,Qun Yi
Among clean energy transformation devices, fuel cells have gained special attention over the past years; however, advancing appropriate non-valuable metal impetuses to halfway supplant the customary Pt/C impetus is still in progress. In this paper, we propose a specific electrocatalyst in the formula of highly-active Cu species, associated with coated carbon (Cu@C-800), for oxygen reduction reaction (ORR) through post-treatment of a self-assembled precursor. The optimized catalyst Cu@C-800 showed excellent ORR performance (i.e., the onset potential was 1.00 V vs. RHE, and half-wave potential of 0.81 V vs. RHE), high stability, resistance to methanol, and high four-electron selectivity. The enhancement is attributed to the synergy between the carbon matrix and a high explicit surface region and rich Cu nano-species.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
ENERGY CONVERSION AND MANAGEMENT
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2021
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IF 9.709
Wen Tang,Jing-Pei Cao,Zhi-Hao Wang,Zi-Meng He,Tian-Long Liu,Ze-Ying Wang,Fei-Long Yang,Jie Ren,Xiao-Yan Zhao,Xiao-Bo Feng,Hong-Cun Bai
The development of cheap and highly dispersed nano-catalyst is one of the key technologies for low temperature steam reforming (SR) of biomass tar. This work used acid-washed and oxidized Shengli lignite char (OXAWSL) as carbon precursor to load Co (Co/OXAWSL) and Ni (Ni/OXAWSL) via ion exchange method to SR of toluene and biomass tar. The Co/OXAWSL was more active and stable than Ni/OXAWSL during the 30 h test with a final toluene conversion of 85% at a relatively low temperature of 450 °C and steam to carbon ratio (S/C) of 3.4, which resulted from its small particle size (5.6 nm) and high dispersion (12.3%) of Co. The relatively high H 2 production (42.59 mmol/g-biomass) over Co 0.1 /OXAWSL (450 °C, S/C = 3.4) in SR of tar was also obtained. A low E a (22.0 kJ/mol) value of Co/OXAWSL and good affinity to oxygen for Co explained its excellent performance. The low-temperature tar cracking process can provide theoretical and technical support for the large-scale industrial utilization of biomass pyrolysis and gasification.
研究领域:
能源科学
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催化化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yanyan An,Mengxin Han,Huaili Zheng,Wei Ding,Qiang Sun,Chao Hu,Liushi Zheng
In heterogeneous reactions, efficient solid–liquid separation of catalyst from water after oxidation is a significant approach to reduce possible secondary pollution of aquatic environments. In this work, a hollow-structured self-floating copper-loaded catalyst (HSM-N-Cu) was fabricated using copper ammonia complexes and hollow glass microsphere as the copper source and supporter, respectively. The SEM, TEM, BET, XPS, and XRD characterization results suggested ideal specific surface area and stability of HSM-N-Cu. The prepared HSM-N-Cu in conjunction with sulfite have been successfully applied for As(III) oxidation in near-neutral conditions. In general, HSM-N-Cu effectively activating S(IV) process involved Cu(II)/Cu(I) conversion and chain reactions of oxysulfur radicals, where the S(IV) acted as a complexing ligand to Cu(II) surface and precursor of oxysulfur radicals. SO 4 − was verified as the dominant contributor to As(III) oxidation, the apparent reaction rate constant ( k obs ’ ) for SO 4 − generation was 1.81 ± 0.12 M −1 s −1 , and the reaction rate constant ( k 12 ) of SO 5 − + As(III) → As(IV) + SO 5 2− was first calculated as 2.6 × 10 6 M −1 s −1 by kinetic study. The apparent activation energy ( E a ) was 48.6 ± 0.1 kJ mol −1 at 100 mg L −1 HSM-N-Cu. Additionally, self-floating HSM-N-Cu could be easily separated, and its great stability was proven after six-cycle test. Furthermore, the HSM-N-Cu/S(IV) system can work effectively in broad range of geochemical conditions. In summary, the established process is feasible for remediation of As(III)-contaminated water, the collection of self-floating catalysts by surface separation from water provides a new idea to reduce secondary pollution of water by catalysts.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 29
·12522-12530
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IF 3.288
Yongdong Chen,Qiang Tang,Zhongbin Ye,Yue Li,You Yang,Haoyu Pu,Gao Li
In this paper, a series of ZnxCe1−xO2 (x = 0.00, 0.05, 0.10, 0.15, and 0.20) nanoparticles were synthesized via an aqueous-phase coprecipitation method. The ZnxCe1−xO2 nanoparticles were coated on honeycomb ceramics to prepare monolithic catalysts, and the catalytic activity of the monolithic catalysts was investigated for the direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol in a continuous tubular fixed-bed reactor. The as-prepared catalysts were fully characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), N2 adsorption/desorption isotherms, H2-temperature-programmed reduction (H2-TPR), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and CO2-temperature-programmed desorption (CO2-TPD). The characterization results showed that doping Zn ions into the ceria lattice formed a fluorite-like solid solution and modified the structure and surface properties of the catalysts. Among all the monolithic ZnxCe1−xO2 catalysts, the monolithic Zn0.10Ce0.90O2 catalyst showed the highest catalytic activity with a methanol conversion of 20.5% with DMC selectivity of 82.1% at 160 °C and 2.4 MPa in the absence of any dehydrating agents. This superior catalytic activity was mainly attributed to a series of better properties, such as larger specific surface area (i.e. 179.9 m2 g−1), higher oxygen vacancy concentration, and the unique structure of the monolithic catalyst (e.g., removing by-product of water in time). This study provides a valuable design strategy for highly efficient direct synthesis of DMC using monolithic catalysts in the fixed-bed reactor.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2016
·Vol. 26
·期 27
·4839-4847
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IF 11.382
Yuanyuan Wu,Guo-Dong Li,Yipu Liu,Lan Yang,Xinran Lian,Tewodros Asefa,Xiaoxin Zou
Making highly efficient catalysts for an overall water splitting reaction is vitally important to bring solar/electrical-to-hydrogen energy conversion processes into reality. Herein, the synthesis of ultrathin nanosheet-based, hollow MoO x /Ni 3 S 2 composite microsphere catalysts on nickel foam, using ammonium molybdate as a precursor and the triblock copolymer pluronic P123 as a structure-directing agent is reported. It is also shown that the resulting materials can serve as bifunctional, non-noble metal electrocatalysts with high activity and stability for the hydrogen evolution reaction (HER) as well as the oxygen evolution reaction (OER). Thanks to their unique structural features, the materials give an impressive water-splitting current density of 10 mA cm −2 at ≈1.45 V with remarkable durability for >100 h when used as catalysts both at the cathode and the anode sides of an alkaline electrolyzer. This performance for an overall water splitting reaction is better than even those obtained with an electrolyzer consisting of noble metal -based Pt/C and IrO x /C catalytic couple—the benchmark catalysts for HER and OER, respectively.
研究领域:
材料科学
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化学工程
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）