CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiangyu Jia,Kai Yuan,Guofu Wang,Shanhui Zhu,Mei Dong,Jiamin Wang,Xiaoming Li,Weibin Fan
Selective reduction of 5-hydroxymethylfurfural (HMF) to valuable 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF) remains a significant challenge under mild conditions. The synergistic effect between metal single atoms (SAs) and nanoparticles (NPs) can greatly enhance catalytic activity. Here, a high-performance Pd SAs catalyst supported on N-doped carbon (PdSAs/NC) was developed from Pd@UiO-66-NH 2 . It was found that partial Pd SAs were spontaneously restructured into Pd NPs during the reaction. Our catalyst exhibited 100 % conversion of HMF and 98 % selectivity towards BHMTHF at temperature as low as 0 °C. In situ FTIR spectra results and density functional theory calculations indicate that Pd SAs contribute to the C = O activation, while Pd NPs facilitated the H 2 dissociation into H* atoms, resulting in synergistic catalytic activity between Pd SAs and Pd NPs.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
You Shu,De-Xuan Xiang,Man-Ying Li,Xiao-Ru Xie,Qing-Yao Chen,Yi-Ting Lin,Zhi-Yong Yang,Yue-jun Ouyang,Gui Chen
Lignin is an important organic polymer and a potential renewable resource. In this work, two novel palladium immobilized on lignin-based hypercrosslinked polymers were successfully fabricated via the Friedel-Crafts alkylation reaction and metallization. The protocol is associated with mild conditions, low cost, high yield, easy separation. The structure of the catalysts were studied by FT-IR, N 2 sorption, XPS, ICP, TGA, TEM, and SEM. Analysis indicates that the polymers exhibit significant characteristics such as large pore volume, highly distributed palladium, excellent chemical and thermal stability, and high specific surface areas. Subsequently, the heterogeneous catalysts were deployed within the context of the Suzuki-Miyaura reaction as a means to evaluate their catalytic activity. In the realm of aqueous environments, HCP-L&Pd-I showcases remarkable efficiency in catalyzing the Suzuki-Miyaura reaction, which benefited from the synergistic effect between the hierarchical pore structure in the material and numerous hydroxyl groups in lignin coordinating with palladium. Under optimum conditions, 0.1 mol% Pd content was enough to react with 97 % yield of biphenyl. Moreover, the catalyst was simply regenerated and reused six times without significant activity loss. This protocol perhaps provides a new perspective on the effective preparation of biphenyl aromatic compounds utilizing lignin-based heterogeneous catalysts in the Suzuki-Miyaura reaction.
研究领域:
化学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2024
·
IF 3.7
Yan Li,Sisi Tang,Hang Lei,Yuxia Zhong,Yue-Fei Zhang
In this paper, two adsorbents based on hydrophilic and hydrophobic fumed silica carriers for efficient recovery of palladium were prepared using 1,4,7,10-tetraazacyclododecane as a functional group. These functional adsorbents were characterized by FT-IR, SEM and BET. The effects of pH (2-6), contact time (1-480 min), and temperature (25-55℃) on the adsorption performance were investigated. The concentration of palladium(II) after adsorption was determined by flame atomic absorption spectrometry and the data were analyzed by kinetic, thermodynamic and isotherm fitting. At pH = 4, the adsorption conformed to Pseudo-second-order kinetic model, with rapid adsorption within 2 h and able to reach equilibrium within 5 h. Meanwhile, the Langmuir model was able to better describe the isotherm data, with the maximum adsorption exceeding 140 mg·g -1 . Moreover, the thermodynamic analysis indicated that the adsorption was a heat-absorbing spontaneous process. The combination of XPS and DFT calculations elucidated the adsorption and desorption mechanisms, emphasized the potential of these adsorbents for the recovery of Pd(II) from aqueous solutions, and contributed to the development of sustainable and effective adsorption technologies.
研究领域:
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zijin Pang,Degang Li,Xinru Wang,Xin Huang,Yu-Shi He,Weimin Zhang,Lipeng Zhang
The electrocatalytic dichlorination (EHDC) shows a promising potential to degrade chlorinated phenols (CPs). It is also a green technology in reducing the corresponding hazardous impact on the environment. In this study, we constructed a catalytic structure which was Pd on a TiO 2 array with oxygen vacancies on carbon fibre paper substrate (Pd/TiO 2 /CFP) by a relatively mild route. Due to the presence of the oxygen vacancies, the resulting strong metal-support interaction (SMSI) effect has been identified which featured a redistribution of spatial charge in Pd/TiO 2 . The electron flow from the oxygen vacancies in the TiO 2 to Pd facilitated the adsorption of Pd with 4-chlorophenol (4-CP) and endowed the Pd metal with an improved chemical reaction kinetics even at a low Pd loading. Experimentally, we studied the dependence of pH, concentration of 4-CP, and working potential on the reaction conditions of EHDC. The results showed that the conversion of 4-CP reached 100 % within 180 min with an apparent rate constant of 2.9 × 10 -2 min −1 and the dominant product was phenol (P). The multi-cycle test illustrated that the Pd/TiO 2 /CFP electrode showed superior stability. The results also revealed that the comprehensive catalytic behavior was much better than those of the Pd/CFP and the TiO 2 /CFP electrodes. The density function theory (DFT) calculations indicated that 4-CP was more preferably absorbed on Pd/TiO 2 /CFP than Pd/CFP due to the SMSI assistance. This study provides a valuable guide in the preparation of precious metal-based electrodes for EHDC with a reduced loading and cost but without performance compromise.
研究领域:
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
JOURNAL OF ORGANIC CHEMISTRY
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2023
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IF 3.6
Chenxu Zheng,Zhi-Jiang Jiang,Ke Jin,Qian Wang,Jian-Fei Bai,Gang Xu,Zhanghua Gao
As a representative scaffold of alkaloids, indoles have been extensively subjected to deuteration, but the regioselective C4 labeling has not been achieved due to its low reactivity. In this work, a Pd-catalyzed deuterium labeling at the indole’s C4 position has been developed under the strategy of transient directing, using D2O as a deuterium source. The substituent effect is found to be crucial in facilitating this H/D exchange process, where the reversing C–D bond formation favors an electron-enriched ligation contrary to its C–H halogenation counterpart.
研究领域:
有机化学
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药物化学
✓ 已验证
DOI
PubMed
高影响因子
SYNTHETIC COMMUNICATIONS
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2018
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IF 1.377
Xinyuan Ma,Qiong Mo,Jie Chang,Kai Xie
This paper mainly studied Pd-catalyzed regioselective chlorination of disubstituted 1,2,3-triazoles directed by the 1,2,3-triazole ring. A series of regioselective chlorinated products were synthesized in 47–86% yields using Pd(OAc)2 as a catalyst and CuCl2 as a chlorinated reagent. This method provides a new mean for the synthesis of 1,2,3-triazole halides which combines the formation of C-X bond with C-H activation.
研究领域:
有机化学
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合成化学
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DOI
高影响因子
Catalysts
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2019
·Vol. 9
·期 12
·1061
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IF 3.444
Zhenhua Dong,Pengwei Gao,Yongmei Xiao,Jing Chen,Wentao Wang
We reveal the Suzuki–Miyaura reaction catalyzed by a Pd–Co nanocatalyst supported by Mg–Fe–CHT (calcined hydrotalcites). A variety of boronic acids and aryl halides were transformed into functionalized biphenyls in excellent yields using water as a solvent. The reaction could proceed under mild conditions with a simple operation and high turnover numbers. The excellent catalytic activities are reasonably attributed to the Co-doping, which forms a Pd–Co alloy on the surface of CHT.Keywords:Suzuki–Miyaura reaction;water solvent;nanocatalyst;palladium;cobalt
研究领域:
化学
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催化材料科学
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2017
·Vol. 31
·期 12
·e3854
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IF 2.319
Xiaojun Ma,Guanghui Lv,Xu Cheng,Weijian Li,Rui Sang,Yong Zhang,Qiantao Wang,Li Hai,Yong Wu
An environmentally friendly palladium(II) catalyst supported on cyclodextrin-modified h-BN was successfully prepared. The catalyst was characterized by FT-IR, SEM, TG, XRD and XPS, and the loading level of Pd in h-BN@β-CD@Pd(II) was measured to be 0.088 mmol g −1 by ICP. It exhibits excellent catalytic activity for the Suzuki and Heck reactions in water, and can be easily separated and consecutively reused for at least nine times. In addition, a series of pharmacologically interesting products were successfully synthesized using this catalyst to demonstrate its potential applications in pharmaceutical industries. Above all, this work opens up an interesting and attractive avenue for the use of cyclodextrin-functionalized h-BN as an efficient support for hydrophilic heterogeneous catalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 53
·33202-33207
·
IF 3.361
Wen Wen,Zhongping Li,Xu Wang,Xiaoyan Du,Guangming Wen,Li Li
Metal nanoclusters (NCs) have recently emerged as a novel class of luminescent nanomaterials and held significant potential in analytical chemistry. In this work, novel polyethyleneimine stabilized palladium nanoclusters (PEI–Pd NCs) were synthesized by chemical reduction at 60 °C for 6 h, and used as a fluorescent nanosensor for the detection of oxytetracycline (OTC). The spectral characteristics, surface structure and morphology of the Pd NCs were studied. The selectivity and stability of the nanosensor were also investigated. The experimental results showed that the Pd NCs had good biocompatibility, stability and photobleaching resistance in aqueous solution. The fluorescence quenching effect showed a good linear relationship with the degree of fluorescence quenching of Pd NCs and OTC in the range of 25–440 nM, with a correlation coefficient of 0.99. The limit of detection (LOD) of the proposed nanosensor for OTC was calculated to be 22 nM. The mechanism of determination was thought to be an inner filter effect (IFE) between OTC and Pd NCs. Based on this, we have established a new nanosensing analysis method for detecting OTC.
研究领域:
分析化学
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纳米材料科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yang Xiao,Chao Qu,Jingjing Zhang,Xi Chen,Wenjin Wang,Xuelong Zheng,Qing Ye
The dissociation of water is essential to water gas shift (WGS) reaction, and the presence of oxygen vacancies can facilitate this key step. Herein, a series of perovskite supported Pd single atoms catalysts were prepared via deposition precipitation method. The incorporation of Pd single atoms can effectively promote the formation of oxygen vacancy on the surface of the catalyst, improving the low temperature reducibility, the ratio of Mn 4 + /Mn 3+ and O ads /O lat compared with support. Among all samples, 0.82 Pd/La 0.5 Ca 0.5 MnO 3 /SBA-15 with the most oxygen vacancies presented 83.6 % CO conversion at 400 °C, specific reaction rate (0.54 mol CO g Pd −1 h −1 ), and TOF (3.77✕10 −2 s −1 ). DFT calculation proved that Pd doping can effectively decreased energy barrier of H 2 O dissociation, and promoted the formation of oxygen vacancies. This work provides experimental and theoretical insights into the rational design of highly active perovskite supported Pd single atom catalysts for WGS reaction.
研究领域:
催化化学
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材料科学
·
理论计算
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yijin Shu,Junjie Shao,Xiaoqiong Wu,Jingwen Tan,Siyao Zeng,Xingfa Zi,Zhijun Chen,Yao Zhang,Xiaoxue Song,Yongtai He,Qijie Mo,Qingsheng Gao
Chevrel phase (CP) molybdenum sulfides (Mo 6 S 8 ) have attracted extensive research attention in the field of energy conversion and storage due to their unique electronic structures and rich open channels. However, comprehensive understanding of intrinsic kinetic mechanisms governing the electrocatalytic bi-functional hydrogen evolution reaction (HER) and hydrogen peroxide (H 2 O 2 ) sensing on CP-based composites is still lacking. Herein, nanosized palladium (Pd) and Mo 6 S 8 particles were assembled in carbon nanowires (C NWs) via electrospinning followed by pyrolysis. The as-obtained novel Pd-Mo 6 S 8 /C NWs exhibited excellent performance in terms of a low overpotential of −194 mV at η 10 for HER, and an ultrahigh sensitivity of 2231 μA mM −1 cm −2 with a limit of detection of 25 nM for H 2 O 2 sensing. The experimental and theoretical findings demonstrated that Pd and Mo 6 S 8 nanoparticles (NPs) exhibited exceptional catalytic activity and strong electronic interactions. The synergistic effects of these two components could effectively modulate the binding strength of reactants and intermediates on the catalyst surface, ultimately leading to improved electrochemical catalytic performance toward reduction of small molecules. Moreover, verification of the stable tolerance in various environments and good selectivity of the electrocatalyst promoted the further use of Pd-Mo 6 S 8 /C NWs-based electrochemical sensing system for sensing additional H 2 O 2 in milk samples, proving the widespread potential of this material for practical applications. This study significantly advances the understanding of nanoscale and bi-functional CP-based composites.
研究领域:
材料科学
·
电化学
·
能源转换与存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemNanoMat
·
2024
·
IF 2.6
Jiangnan Guo,Shuozhen Hu,Xinsheng Zhang,Shigang Sun
Utilizing carbon coated ferroelectric materials to introduce polarization-induced electric field (PIEF) stimulates research of electric field-assisted catalysts for various reactions. However, effect of PIEF on carbon coating mechanism has not been studied. Herein, tourmaline nanoparticles (TNPs) with spontaneous dipole moments were applied as the PIEF supplier and sucrose was utilized as the carbon precursor to synthesize carbon coated TNPs (TNP@SC) to uncover the influence of PIEF on the carbon coating and catalytic activity of Pd toward formic acid decomposition (FAD). PIEF enhanced the adsorption capacity of TNPs for the caramelized intermediate species and increased H+ concentration by facilitating water ionization. Polymerization of adsorbed caramelized intermediate species on TNPs was accelerated. Uniformly coated carbon layer with more defects, larger specific surface area, and higher porosity was coated on TNP. Such surface properties of the carbon layer were beneficial for strongly anchoring ultrafine Pd nanoparticles. Owing to the specific properties of carbon layer and existence of PIEF, Pd/TNP@SC exhibited higher FAD activity than the catalysts absent of PIEF. Stronger PIEF leaded to higher initial turnover frequency. This study provides guidance to supply electric field for catalysis.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
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