INORGANIC CHEMISTRY COMMUNICATIONS
·
2019
·
IF 1.795
Yanjie Zhou,Wei Wei,Hua Su,Wei Wang
Developing a sensitive and reliable method for accurate determination of H 2 is of great importance for effective and safe utilization of H 2 in various conditions. A fluorescence (FL) assay for H 2 detection was proposed in the present work. It relied on the fact that Pd/C nanocomposites catalyzed fluorogenic conversion of weakly-FL resazurin (RZR) into highly-FL resorufin (RSR) was triggered by H 2 under ambient condition. This method possessed a limit of detection (LOD) as low as 0.06% volume concentration of H 2 in air, far below 4% that is the generally recognized as the lower explosion limit of H 2 -air mixture. A high selectivity to H 2 over O 2 , N 2 , Ar and CO 2 as well as broad linear response range from 0.2% to 80% made this method promising for H 2 sensing in a variety of circumstances. Most importantly, the developed method was able to detect practical H 2 atmosphere (2% H 2 in air) with high reliability under simple operation.
研究领域:
化学
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材料科学
·
分析化学
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DOI
高影响因子
Nanomaterials
·
2025
·Vol. 16
·期 1
·
IF 4.3
Yu Zhang,Ying Xin,Lizheng Tang,Shihao Cui,Hongling Duan,Qingshan Zhao
The selective hydrogenation of phenol to cyclohexanone is a pivotal reaction for producing nylon precursors. Conventional Pd/C catalysts, however, suffer from weak metal–support interactions, leading to size heterogeneity and agglomeration of Pd nanoparticles, which degrades their activity and stability. Herein, we report a facile argon plasma treatment to engineer rich defects on an activated carbon (AC) support, resulting in a highly dispersed and stable catalyst (denoted as PL-Pd@ACAr). Characterization results indicate that the abundant carbon defects in PL-Pd@ACArenhance the anchoring of Pd precursors, ensure the uniform dispersion of Pd nanoparticles, and effectively modulate their electronic structure. Consequently, the plasma-enabled PL-Pd@ACArcatalyst achieves 99.9% phenol conversion with 97% selectivity to cyclohexanone at a mild temperature of 70 °C and maintains exceptional stability over six consecutive cycles. This work provides a robust and efficient strategy for the surface engineering of carbon supports to design high-performance hydrogenation catalysts.
研究领域:
催化化学
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材料科学
·
化学工程
·
绿色化学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Jiangtao He,Xinwei Wang,Ming Gao,Yugang Su,Hongsheng Jia
Magnesium hydride (MgH 2 ) suffers from sluggish kinetics and high operational temperatures, hindering practical hydrogen storage. We pioneer a spatially decoupled catalytic strategy that assigns distinct roles to Ti 0 . 10 Zr 0 . 15 V 0 . 35 Cr 0 . 10 Ni 0 . 30 (TA) alloy (bulk diffusion promoter) and Pd/C (surface dissociation catalyst), overcoming the inherent coupling of rate-limiting steps in MgH 2 . This design achieves near-ambient absorption (4.56 wt% at 100 °C) and eliminates activation cycles—a milestone unattained by single-catalyst systems. Kissinger analysis confirms a 46.0% reduction in activation energy (78.8 kJ/mol) for the surface-limited step, directly validating the spatial separation of catalytic functions. Crucially, the composite retains 92.3% capacity after 30 cycles with negligible kinetic degradation (0.40% decay/cycle), eliminating the need for activation. This work establishes a spatially coupled catalytic mechanism that decouples surface and bulk processes, enabling a lower operating temperature for MgH 2 .
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DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2015
·
IF 3.564
Xiao-ning Ye,Qiang Lu,Wen-tao Li,Pan Gao,Bin Hu,Zhi-bo Zhang,Chang-qing Dong
A new technique was proposed to selectively produce nicotyrine, a valuable alkaloidal product, from catalytic fast pyrolysis of tobacco mixed with the Pd/C catalyst. Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were performed to investigate the effects of pyrolysis temperature and catalyst-to-tobacco ratio on the selective nicotyrine production. The actual nicotyrine yields under different reaction conditions were quantitatively determined. Moreover, the catalytic activity of the Pd/C catalyst was compared with those of the activated carbon (AC), Ru/C and Pd/SBA-15 catalysts. The results indicated that during the catalytic fast pyrolysis process, the Pd/C catalyst possessed promising dehydrogenation capability to selectively convert the nicotine in tobacco into the nicotyrine, and it performed much better than the other three catalysts. The maximal nicotyrine yield reached as high as 2.80 wt%, obtained at the pyrolysis temperature of 400 °C and catalyst-to-tobacco ratio of 2.
研究领域:
能源与环境科学
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化学工程
·
植物化学
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产品关联
DOI
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 7
·e18085
·
IF 3.7
Wei Wang,Baian Pu,Chi Ma,Chengxiang Shi,Lun Pan,Xiangwen Zhang,Ji-Jun Zou
Cyclopropane derivates are appealing to synthesis of high-energy-density fuels because of the high strained energy of the three-numbered ring. The catalytic cyclopropanation of olefin with diazomethane is very effective to construct the carbocycle. The majority of the catalysts employed are nonrecyclable homogeneous compounds. Herein, we report cyclopropanation of polycyclic olefins catalyzed by heterogeneous Pd/C. The optimal cyclopropanation conditions were explored utilizing dicyclopentadiene as model substrate and a series of polycyclic olefins were cyclopropanated with high yield. Additionally, the catalyst has good recyclability and stability, as shown by characterizations as well as the fact that no inactivation happens after cyclopropanation. The synthesized cyclopropane derivates exhibit good fuel characteristics like high density (1.006–1.087 g/cm 3 ), high volumetric net heat of combustion (42.58–46.45 kJ/cm 3 ), good low-temperature and combustion performance. This work shows industrial potential for cyclopropanation of polycyclic olefins with diazomethane.
研究领域:
化学工程
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能源科学
·
催化材料
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 13
·4741-4752
·
IF 10.182
Song Li,Qiaozhi Ma,Wenxin Zhong,Xuelai Zhao,Xiangqian Wei,Xinghua Zhang,Qiying Liu,Chenguang Wang,Longlong Ma,Qi Zhang
Catalytic hydrodeoxygenation of bioderived furans is critically attractive to prepare sustainable fuels. Herein, a novel octanediol-route was developed to produce octane through one-pot conversion of bioderived furans at low temperatures. A 96.6% yield of octane was obtained by catalytic conversion with Pd/C and phosphotungstic acid (HPW). Experimental validation of the novel pathway revealed that octanediol intermediates could be formed through hydrogenolysis of furans before deoxygenation. The spontaneous process of this octanediol-route was thermodynamically confirmed by DFT simulations. In addition, characterization studies suggested that water in the system strengthened the cooperation between metals and acids to facilitate C–O bond scission through the modification and hydrogen transfer of HPW. This work highlights a promising reaction pathway for an efficient HDO catalytic system to obtain alkanes from bioderived furans under mild conditions.
研究领域:
催化
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可持续化学
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可再生能源
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DOI
高影响因子
ChemistrySelect
·
2026
·Vol. 11
·期 10
·e07382
·
IF 2.3
Tong Zhang,Haiyong Wang,Chenguang Wang,Chen Shen,Qiying Liu
Monohydric alcohols are important platform molecules with diverse applications in organic synthesis, pharmaceuticals, food, and polymer industries. The production of monohydric alcohols via the selective hydrogenolysis of diols holds significant scientific and practical value. However, the precise catalytic control of the cleavage of target C–C and C–O bonds remains an open challenge, which often leads to low yields of the target products. Herein, metal-acid bifunctional catalysts were employed to boost the conversion of diols and improve the production of monohydric alcohols through hydrogenolysis. By regulating key reaction intermediates, a maximum yield of 76.2% for 1-propanol and a total monohydric alcohol yield of 84.9% were achieved within a short reaction time of 1 h. Our investigations demonstrate that the composite system of 5% Pd/C and phosphotungstic acid (HPW) catalyzes the conversion of ethylene glycol (EG) and 1,2-propanediol via a metal-acid synergistic effect, which enables the selective cleavage of C–C and C–O bonds. Ethylene glycol and 1,2-propanediol were thus converted to the monohydric alcohols (ethanol, n-propanol, and isopropanol) through hydrogenolysis and dehydration-hydrogenation processes. Additionally, the reaction order and activation energy barriers for the conversion of diols over the 5% Pd/C catalyst were determined experimentally. This work establishes a preliminary method for the production of monohydric alcohols from the hydrogenolysis of small-molecule diols by 5% Pd/C and HPW catalysts. Given the commercial availability of these catalysts, the developed catalytic system exhibits promising practical application potential and may facilitate the scale-up of this reaction. Graphical A 5% Pd/C–phosphotungstic acid (HPW) composite catalyzes the conversion of ethylene glycol and 1,2-propanediol via metal–acid synergy, enabling selective C–C/C–O cleavage. Hydrogenolysis and dehydration–hydrogenation yield ethanol, n-propanol, and isopropanol. Reaction orders and activation energies were determined, linking mechanistic insights to industrial scale-up for biomass diol upgrading.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Yaxing Li,Rui Zhang,Xianghai Meng,Ping Ouyang,Haiyan Liu,Chunming Xu,Zhichang Liu
Acid-soluble oil (ASO) was produced during isobutane alkylation catalyzed by chloroaluminate ionic liquids (CAILs). However, the ASO composition characterizations and deactivated CAIL regeneration pathway were not clarified. In this work, a series of characterizations (elemental analysis and infrared, ultraviolet, and mass spectroscopy) were performed to reveal the ASO composition. The result showed that ASO contained numerous conjugated cycloolefins with various alkyl substituents and a few O1–O5 compounds. The activity index (AI) value of fresh CAILs was 1.74 and decreased to 1.18 with the addition of 9.09 wt % ASO because the [Al2Cl7]− anion in CAILs was complexed by C═C and C═O bonds in ASO. The hydrogenation regeneration of deactivated CAILs on the Pd/C catalyst was studied. The AI value of regenerated CAILs increased to 1.45 because unsaturated bonds in ASO were hydrogenated to saturation. Recovery of unsaturated hydrocarbons followed the order benzene > 1-methylcyclopentene > pentamethylcyclopentadiene. This work demonstrated that low ASO recovery was attributed to the partial occupation of the π-electron of unsaturated bonds by the [Al2Cl7]− anion.
研究领域:
化学工程
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催化
·
石油化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Hui Chen,Jie He,Jinsheng Sun
The production of cyclohexanone, of industrial importance, is at a distance to environment friendly and efficiency. As a solution, a mild sustainable catalytic hydrogenation is presented herein, of phenol into cyclohexanone on Pd/C with potassium formate the hydrogen donor under open atmosphere. Some important reaction conditions, such as temperature, reaction time, catalyst, amount of potassium formate, etc. were investigated and analyzed. The positive growth was found to accelerate the conversion rate of phenol while reducing cyclohexanone selectivity by weakening the protection of phosphotungstic acid. Phosphotungstic acid was confirmed to be the co-catalyst exhibiting the highest activity under given conditions. Based on experiments, we have made reasonable assumptions about the reaction mechanism, while the reaction kinetics proves high reaction rates within a wide temperature range, indicating the reaction to be quick process. Furthermore, the good reusability and recyclability of Pd/C catalyst is verified to benefit future industrial applications.
研究领域:
化学工程
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yuan Li,Biao Pei,Junjie Chen,Shaosuo Bing,Linxiao Hou,Qi Sun,Gang Xu,Zhikan Yao,Lin Zhang
A novel catalyst with a yolk-shell structure was designed to overcome the leaching of noble metals in heterogeneous catalysis. Through a template method, palladium (Pd) nanoparticles were encapsulated by hollow spherical covalent organic frameworks (COFs) consisting of 2,4,6-trihydroxybenzene-1,3,5-tricarbaldehyde (Tp) and p-phenylenediamine (Pa). The final catalyst with a yolk-shell structure was denoted as (Pd/C)@TpPa COFs. The unique morphology and chemical structure of this novel composite (Pd/C)@TpPa COFs were confirmed by a transmission electron microscope (TEM), a laser particle analyzer, X-ray diffraction (XRD), and N 2 adsorption and desorption. Subsequently, to demonstrate its catalytic performance brought by structural design, this novel catalyst was applied to catalyze the Suzuki reaction . Interestingly, this catalyst exhibited a brilliant size cutoff efficiency for aryl benzene amounting to 100% and achieved a high conversion with only 0.05 mol% Pd loading. Besides, this catalyst could be readily recovered via filtration and reused for at least five consecutive cycles without any significant loss in its activity.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Lanlan Shi,Xiaojun Wang,Feike Zhang,Jingxian Li,Yuanming Liu,Weijie Fu,Shuyun Yao,Shiyu Wang,Kang Ji,Yingjie Ji,Zhiyu Yang,Liwen Zhang,Jiangzhou Xie,Yi-Ming Yan
Palladium metal catalysts have emerged as the preferred choice for alkaline formate oxidation reaction (FOR) due to their high activity. However, their strong binding with adsorbed H (Had) allows Had to occupy the active site, resulting in slow FOR kinetics. Herein, we developed a ZrO2/Pd/C catalyst to decrease the Had binding strength on Pd active sites, thereby enhancing the FOR in alkaline media. Through experimental investigations and density functional theory (DFT) calculations, we elucidated the relationship between the d-band center of Pd and hydrogen binding energy (HBE). Our findings reveal that electron transfer from ZrO2 to Pd, driven by the work function disparity, results in a downshift of the d-band center of Pd. This shift weakens the HBE at Pd active sites, facilitating the desorption of Had intermediates and thereby improving catalytic efficiency. As a result, the ZrO2/Pd/C catalyst demonstrated a 2.8-fold increase in activity over commercial Pd/C, exhibiting a lower peak potential and a significantly higher peak current of 1787 mA mg–1. This work advances our understanding of the interplay between electronic structure and catalytic performance, setting a benchmark for high-performance electrocatalysts in energy conversion technologies.
研究领域:
催化
·
电化学
·
材料科学
·
能量转换
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Jianfeng Lin,Xuri Wu,Yijun Chen
Statins, leading cholesterol-lowering drugs, contain a pivotal pharmacophore side chain. However, the Pd/C-catalyzed debenzylation step in the side chain production poses a series of cost and environmental issues. In this study, an efficient debenzylase is generated from the engineering of CYP102A1 to replace the tedious and harmful chemical debenzylation. The engineering process for the debenzylase is primarily enabled by continuous dynamic protein conformational alteration-guided mutagenesis, a newly developed protein dynamics-based strategy to facilitate the prediction of the key residues of both proximal and challenging distal sites, for the improvement of activity and selectivity. Through iterative combinatorial mutagenesis, the best mutant exhibits a 22.6-fold improvement in the total turnover number and an increase in the debenzylating selectivity from 12.2% to 99.8%. Furthermore, the practical value of the debenzylase is demonstrated by incorporating a diketoreductase-mediated synthetic route through an enzymatic cascade reaction to produce an advanced precursor of statins. This study not only establishes the first enzymatic alternative to the removal of the widely used benzyl group in organic synthesis but also paves the way for accelerating enzyme engineering in a rational manner.
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DOI
高影响因子