ChemSusChem
·
2024
·Vol. 17
·期 16
·e202400637
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IF 7.5
Peixin Wang,Wenhua Xue,Jian Ye,Ruilong Zhang,Reeti Kumar,Wenfei Cai,Jun Zhao
Graphical A catalyst for the thermal catalytic reaction of glucose isomerization to fructose that can be regenerated through light illumination. The isomerization of glucose to fructose plays a crucial role in the food industry and the production of biomass-derived chemicals in biorefineries. However, the catalyst used in this reaction suffers from low selectivity and catalyst deactivation due to carbon or by-product deposition. In this study, MgSnO 3 catalyst, synthesized via a facile two-step process involving hydrothermal treatment and calcination, was used for glucose isomerization to fructose. The catalyst demonstrated outstanding catalytic performance, achieving a fructose equilibrium yield of 29.8 % with a selectivity exceeding 90 % under mild conditions owing to its acid-base interaction. Notably, spent catalysts can be regenerated by photoirradiation to remove surface carbon, thereby avoiding the changes in properties and subsequent loss of activity associated with conventional calcination regeneration method. This novel approach eliminates the energy consumption and potential structural aggregation associated with traditional calcination regeneration methods. The acid-base active sites of the catalyst, along with their corresponding catalytic reaction mechanism and photoregeneration mechanism were investigated. This study presents a demonstration of the comprehensive utilization of catalytic material properties, i. e., acid-base and photocatalytic functionalities, for the development of a green and sustainable biomass thermochemical conversion system.
研究领域:
化学工程
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可再生资源与环境科学
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DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2022
·
IF 11.072
Jiajin Huang,JiaYu Chen,Jinze Yao,Siyao Zhao,Xingbei Wu,Qibin Xia
The challenge for selective catalytic reduction (SCR) of NO x with NH 3 is to improve de-NO x activity at low temperatures while simultaneously improving the tolerance of catalysts towards SO 2 poisoning. Herein, V and Ce oxides were loaded on deactivated SCR catalysts subjected to acid pickling (CAT) via impregnation to recover de-NO x activity. The resulting V–Ce@CAT catalyst exhibited 85–95% NO x conversions over a wide temperature window of 200–450 °C while conversions of only 40–78% over the same temperature range were observed with CAT (spent catalyst treated with acid). Interestingly, in addition to the high tolerance towards SO 2 displayed by V–Ce@CAT, the catalyst exhibited improved reactivity after the introduction of 200 ppm SO 2 , with the NO x conversion increasing from 80% to 87%. The results indicated that a kinetic equilibrium was reached between the formation and decomposition rates of Ce 2 (SO 4 ) 3 on V–Ce@CAT which prevented the accumulation of surface sulfate species, thereby protecting the main active species V from catalytic inactivation. Furthermore, in situ DRIFTS revealed that the NH 3 -SCR reaction pathway of V–Ce@CAT follows the L-H mechanism.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2016
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IF 2.628
Xinping Duan,Yan Yin,Xuelin Tian,Jinhuo Ke,Zhaojun Wen,Jianwei Zheng,Menglin Hu,Linmin Ye,Youzhu Yuan
Disintegration or redispersion of supported sintered gold nanoparticles (Au NPs) in the presence of alkyl halide can give catalyst regeneration or redispersion of sintered Au catalysts. The selectivity of alkyl halides, temperature and size distributions were investigated to elucidate the redispersion of Au NPs during halide-induced decomposition. This study proved that the alkyl halide induced the redispersion of sintered Au NPs which depended on the R–X (X = I, Br, Cl) bond dissociation energy (BDE) and thus provided a simple descriptor for the regeneration of inactive supported Au catalysts. A correlation between the BDE of R–X and dispersion efficiency was established. The tendency for disintegration and redispersion followed the R–X BDE of the alkyl halide. Compared to alkyl chlorides and bromides, iodides were more efficient for redispersing sintered Au NPs. As a descriptor, the BDE of R–I played a crucial role in particle redispersion. These findings provided insights into the mechanism of organic halide-induced Au NP disintegration and the effect of the halide type on the redispersion of sintered catalysts.
研究领域:
化学
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催化科学
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DOI
高影响因子
iScience
·
2021
·
IF 5.458
Mingwei Weng,Zihao Zhang,Francis Okejiri,Yue Yan,Yubing Lu,Jinshu Tian,Xiuyang Lu,Siyu Yao,Jie Fu
Catalytic transfer hydrogenation (CTH) of biomass-derived furfural (FAL) to furfuryl alcohol is recognized as one of the most versatile techniques for biomass valorization. However, the irreversible sintering of metal sites under the high-temperature reaction or during the coke removal regeneration process poses a serious concern. Herein, we present a silicalite-1-confined ultrasmall CuO structure (CuO@silicalite-1) and then compared its catalytic efficiency against conventional surface-supported CuO structure (CuO/silicalite-1) toward CTF of FAL with alcohols. Characterization results revealed that CuO nanoparticles encapsulated within the silicalite-1 matrix are ∼1.3 nm in size in CuO@silicalite-1, exhibiting better dispersion as compared to that in the CuO/silicalite-1. The CuO@silicalite-1, as a result, exhibited nearly 100-fold higher Cu-mass-based activity than the CuO/silicalite-1 counterpart. More importantly, the activity of the CuO@silicalite-1 catalyst can be regenerated via facile calcination to remove the surface-bound carbon deposits, unlike the CuO/silicalite-1 that suffered severe deactivation after use and cannot be effectively regenerated.
研究领域:
化学工程
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材料科学
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DOI
PubMed
高影响因子
STAR Protocols
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2024
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IF 1.3
Xinze Du,Yumei Liu,Xiaojun Shen
Summary Phenolic chemicals are important building blocks in chemical and material industries. In this protocol, we describe the preparation of CeO 2 -CuO catalysts and the application in the decarboxylative oxidation reaction of benzoic acids to phenols. Furthermore, we describe how to modify the basic sites of CeO 2 -CuO catalysts by CO 2 treatment to increase the selectivity of phenol and the regeneration process of used catalyst. For complete details on the use and execution of this protocol, please refer to Du et al. (2023). 1
研究领域:
催化
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有机化学
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材料科学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Wenying Li,Yongkang Lv,Huazhang Zhao,Jianfeng Li
Electrochemical method has been used to induce peroxymonosulfate (PMS) activation for removing contaminants, yet low PMS activation rate limited its reaction activity. In this study, a microbial fuel cell (MFC) system with CuCo 2 S 4 as cathode catalyst for PMS activation (PMS/CuCo 2 S 4 -MFC) was established. The results showed that three-dimensional nanoflake structure of CuCo 2 S 4 could provide more active sites for PMS activation and exhibited the excellent electrochemical performance. The apparent degradation rate ( k a ) of Rhodamine B (RhB) in this system was 6.5 times and 1.2 times higher than MFC and CuCo 2 S 4 alone, suggesting that PMS activation was attributed to both CuCo 2 S 4 and electrochemistry in the system. In addition, the decrease of k a over five cycles in the system was approximately 3 times slower than CuCo 2 S 4 alone, indicating that the catalyst stability was improved significantly. This is mainly attributed to the in-situ regeneration of Cu 2+ and Co 3+ through receiving the electrons generated from MFC anode . The radical quenching results indicated that RhB was degraded mainly through the radical pathway, in which sulfate radical was the key reactive species. This study provides an energy-saving approach for PMS activation, which will be useful for further development of PMS-based advanced oxidation process .
研究领域:
环境科学
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电化学
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催化材料
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Jing Gao,Meng Hao,Tao Wu,Yujiang Li
The purpose of this work is to investigate desorption efficiency for regenerating a crude oil-contaminated catalyst by using an ex-situ surfactant/solvent washing technique. We employed six types of surfactants and solvents for optimization, and established an optimal mixture of surfactant and solvent for the removal of crude oil from the contaminated catalyst. The efficiency of the surfactant/solvent mixture for the removal of crude oil from the contaminated catalyst was determined based on the mass ratio of surfactant to solvent, contact time, pH, and temperature. The raw catalyst, crude oil-contaminated catalyst, and after washing catalyst were characterized by interracial rheometer , zeta-potential analyzer, and scanning electron microscope . We found that the Brij-58/1,2-dimethylbenzene mixture could provide superior crude oil removal efficiency. At a higher mass ratio of 1,2-dimethylbenzene, the crude oil removal rate of the contaminated catalyst exceeds 95%. This result is attributed to the addition of the solvent to the surfactant solution. The solvent can significantly decrease the surfactant’s CMC and increase the micelle’s number, thereby enhancing the mixture’s washing efficiency. Since aromatic solvents and crude oil components have similar structures in terms of polarity and aromaticity, the Brij-58/1,2-dimethylbenzene mixed system has a strong affinity for crude oil components.
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
Catalysis Science & Technology
·
2020
·Vol. 11
·期 4
·1497-1509
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IF 5.721
Xiaoyue Wan,Nannan Tang,Qi Xie,Shuangyan Zhao,Chunmei Zhou,Yihu Dai,Yanhui Yang
A CuMn2O4 spinel oxide was prepared via a freezing-assisted sol–gel method and used in the aerobic oxidation of 5-hydroxylmethylfurfural (HMF) toward 2,5-furandicarboxylic acid (FDCA) in aqueous solvent. A highest FDCA yield of 92.1% over the CuMn2O4 spinel oxide was achieved and the catalyst could be regenerated by calcination in air after the sixth consecutive run, outperforming several other Mn-based spinel and single oxide catalysts. Kinetic studies reveal that HMF → 2,5-diformylfuran → 5-formylfuran-2-carboxylic acid (FFCA) → FDCA is the primary reaction route of the reaction and that the oxidation of FFCA is the rate-determining step over the CuMn2O4 spinel. Characterization measurements show that Mn species enrichment and proper Mn4+/Mn3+, Cu2+/Cu+ and Cu/Mn ratios on the surface of the catalyst led to an appropriate Olatt./Oads. ratio, which facilitated oxygen mobility between the Olatt. consumption and the Olatt. generation via the refilling of oxygen vacancies. Synergistic effects between Mn and Cu in the CuMn2O4 spinel inhibit the secondary reaction and accelerate the rate-determining step rate to enhance FDCA formation.
研究领域:
化学工程
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催化化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Jin Chen,Xuelong Lv,Wenjian Xu,Xiaolan Li,Jing Chen,Hongpeng Jia
The exploit of simple method to synthesize and recover catalyst is meaningful to widespread application of environmental catalysis. Different from traditional knowledge about deposition of Ag cation by Cl anion, we find that Cl anion coordinates with Ru and Ag cations simultaneously to micro-micelles and results in homogeneously alloying of bimetals. The Ru-Ag alloy exhibits a remarkable activity and stability in propane catalytic oxidation at moderate condition, but is still inactivated by extremely-high temperature and humidity due to metal sintering and oxidation as well as support reconstruction. Fortunately, utilization of Cl coordination to extract and combine bimetals at redox condition is proved as a feasible and simple way to regenerate the thermally-inactivated catalyst. With in-situ characterization, the synergic effect between Ru and Ag on propane oxidation obeying Mars-van-Krevelen mechanism is revealed. Through monolith test, the practice application of Ru-Ag catalyst prepared via Cl-assisted method is thought to be promising.
研究领域:
催化
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环境化学
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材料科学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2025
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IF 13.1
Jilei Lin,Meiqing Shen,Sifeng Bi,Gurong Shen,Feng Gao,Wei Li
Propylene production via propane dehydrogenation (PDH) over supported platinum (Pt) catalysts is a vital industrial process. However, rapid catalyst deactivation due to coking necessitates periodic regeneration under harsh oxidative conditions. While alloying Pt with transition metals significantly reduces coking, these alloy catalysts often exhibit poor regeneration stability. In this study, we demonstrate that supporting PtIn nanoparticles on Y2O3-modified δ-Al2O3 yields a PDH catalyst with significantly improved activity and stability. This catalyst achieves propane conversion rates close to the thermodynamic equilibrium at an ultralow Pt loading of 0.1 wt %, along with high propylene selectivity. Notably, this catalyst also exhibits remarkable regeneration stability. Through reaction-regeneration cycling experiments with various catalyst formulations, we reveal that the alloy effects between Pt and In are primarily responsible for enhanced catalyst stability under steady-state reaction conditions by suppressing coke formation. Meanwhile, the incorporation of Y2O3 as a support component significantly improves stability during regeneration. Density functional theory (DFT) calculations further elucidate the key factors contributing to the enhanced anticoking properties of the catalyst under PDH reaction conditions.
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高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Dekang Li,Zhixian Bao,Lijun Jin,Haoquan Hu
Dry reforming of methane (DRM) can spontaneously use CO2 and CH4 to produce syngas, but minimal sulfur impurities in the feed gas can poison and deactivate the catalyst. Although the Ni/Al2O3 catalyst has excellent DRM activity, it is challenging to regenerate due to sulfation of the support. Besides that, the loading of sacrificial promoters used to improve sulfur resistance, such as Cu, may impact the DRM performance of active sites. Here, a spatial separation strategy was proposed to precisely design a sulfur-resistant catalyst, dividing the catalyst into a DRM zone and a H2S adsorption zone. The Ni@SiO2@NiCu catalyst prepared by this strategy shows stable DRM performance and significantly improved sulfur resistance and can be regenerated repeatedly. The Ni@SiO2@NiCu catalyst has the best sulfur resistance, 6.8 times that of the spatially adjacent NiCu@SiO2 catalyst and 1.4 times that of the Ni@SiO2@Cu catalyst. This spatial separation strategy introduces a novel concept for the controllable synthesis of sulfur-resistant catalysts and may inspire further applications in the design and development of such catalysts.
研究领域:
催化化学
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化学工程
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材料科学
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环境科学
·
能源技术
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DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2025
·Vol. 236
·期 10
·1-13
·
IF 3
Li Yuan,Fan Jun,Huang Bingyao,Li Hongyan,Zhao Jie,Li Kai,Wang Fei
Removal of PH 3 from industrial gases have attracted extensive attention due to its high toxicity and catalyst poisoning characteristics. In this study, a series of copper-based support-free catalysts were synthesized by a facile method using different nitrogen and carbon sources. The 100% removal of PH 3 could reach 540 min in micro-oxygen environment by using the obtained catalyst. The X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS) results exhibited that the formation of Cu 3 P was contributed to the deactivation of the catalysts, which was considered as active component for the decomposition of PH 3 . The PH 3 decomposition performance could achieve 99% under 450 ℃ with 90% yield of H 2 using the exhausted catalysts. This strategy is beneficial for the development of dephosphorization catalyst and provides a new route for the secondary use of exhausted catalysts. Graphical A facile strategy was employed for synthesize support-free catalysts for PH3 oxidation by using Cu(NO3)2 and different nitrogen resources or carbon resource. The performance were thoroughly compared. The exhausted catalyst was conducted in the PH3 catalytic dissociation reaction, where the conversion rate of PH3 could reach 99% with 90% hydrogen production under 450 ℃.
研究领域:
环境催化
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材料科学
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工业气体净化
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化学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）