Molecular Catalysis
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2022
·
IF 5.089
Jiaoyan Zhu,Tiefeng Xu,Panting Lu,Wenxing Chen,Wangyang Lu
Exploring sustainable catalysts for the transition-metal-catalyzed carbonylation and acknowledging the corresponding interior mechanism are of great interest. Herein, palladium supported spherical-like graphitic carbon nitride catalyst (Pd@s-CN) was prepared through a microwave-assisted approach, where s-CN with larger surface area was synthesized via an exfoliation and refluxing method. The spherical-like structure of s-CN can offer abundant space preventing the agglomeration of Pd and creating more active sites for carbonylation reaction. Notably, with iodobenzene as the substrate, Pd@s-CN achieved 92% yield of benzoic acid, and its performance was better than that of PdCl 2 and Pd/C catalysts. The effects of thermal, light source and catalyst structure were investigated. Ultimately, the reaction mechanism of photocatalytic carbonylation was proposed. This environmentally friendly photocatalytic carbonylation method is expected to provide a new idea for carbonylation and other related organic synthesis reactions.
研究领域:
化学
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材料科学
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催化科学
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产品关联
DOI
高影响因子
Nanoscale
·
2023
·Vol. 15
·期 15
·7032-7043
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IF 6.7
Bowei Pan,Shuang Shan,Junpeng Wang,Quan Tang,Longfei Guo,Tao Jin,Qiao Wang,Zhen Li,Muhammad Usman,Fuyi Chen
The study provides a proof of concept for the first time that unique palladium–gold (PdAu) and palladium–silver (PdAg) nanodendrites are bifunctional catalytic active sites for formate oxidation reactions (FORs) and formate dehydrogenation reactions (FDRs). The unique nanodendritic structure was developed via a simple galvanic displacement reaction for the direct growth of PdAu and PdAg nanodendrites on a nickel foam (PdAu/NiNF and PdAg/NiNF). These PdAu/NiNF and PdAg/NiNF electrodes exhibited 2.32 and 1.59 times higher specific activity than that of the commercial Pd/C electrode and promising stability toward FORs. Moreover, the PdAu/NiNF and PdAg/NiNF nanodendrites were also highly active and selective catalysts for hydrogen generation from a formate solution with turnover frequency (TOF) values of 311 h−1 and 287 h−1 respectively. Impressively, a passive air-breathing formate fuel cell with PdAu/NiNF used as an anode can yield an open-circuit voltage of 1.12 V and a peak power density of 21.7 mW cm−2, which outperforms most others reported in the literature. PdAu and PdAg nanodendritic catalysts supported on a nickel foam demonstrate an open structure and uniform catalyst distribution and offer a promising nanoalloy for air-breathing formate fuel cells and on-site chemical hydrogen production systems.
研究领域:
材料科学
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电化学
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能源科学
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产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
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2022
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IF 4.177
Hang Mei,Zi-Yan Wang,Yue Zhai,Qiang-Qiang Zhu,Le Wang,Pei Liang
Vacancy-ordered double perovskites, the variant of metal-halide perovskites, have excellent potential for use in optoelectronic and thermoelectric devices. A narrow region of forming the stable vacancy-ordered double perovskite Cs2PdBr6 by the chemical potential calculation via the first principles method was reported. Perdew–Burke–Ernzerhof functionals were used to investigate the possible intrinsic defects and the corresponding formation energy of Cs2PdBr6. Under the Pd-rich condition, the VBr defect was spontaneously formed as it has the lowest formation energy among all donor defects. In contrast, the sample became a p-type conducting material with a high hole concentration under the Pd-poor condition. This indicates that the defect-induced decline of photoelectric properties of Cs2PdBr6 can be alleviated by regulating the VBr defect alone. Finally, the Cs2PdBr6 microcrystals were fabricated via hydrothermal synthesis. In addition, XRD, PL, and Raman spectroscopy were also performed on Cs2PdBr6 powder to characterize the microstructure and optical properties of the compound; the results showed that VBr defects can be formed spontaneously, which is consistent with our theoretical calculations.
研究领域:
材料科学
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物理化学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Xu Yin,Jiatian Yu,Zhifeng Gao,Wei Li,Kajia Wei,Yun Jiang,Yonghao Zhang,Haoming Chen,Weiqing Han
Bromate (BrO 3 – ) is a common by-product of advanced oxidation water treatment processes. In this study, a catalyst combining MXene and Pd was synthesized to eliminate BrO 3 – by electrochemical reduction in flow-through mode. The fabricated Ti/Pd@MXene filter showed superior activity for BrO 3 – reduction compared with Ti/MXene filter. A satisfactory BrO 3 − removal performance by Ti/Pd@MXene filter was obtained at pH values of 5–7 with a current density of 1.0–2.5 mA·cm –2 . The mechanism explored by quenching experiments and EPR analysis demonstrated that atomic hydrogen (H*)-mediated reduction was dominant in the Ti/Pd@MXene filter system and contributed to 84.2 % of the BrO 3 − removal, which was greater than that of Ti (7.1 %) and Ti/MXene (43.9 %). DFT calculations revealed the introduction of Pd nanoparticles on MXene lowered the energy barrier for generating H* from OH* -H* , thus boosting H* formation. Furthermore, the Ti/Pd@MXene filter had favorable stability and applicability, and nearly 90 % of BrO 3 − could be eliminated in different water matrices. Moreover, energy consumption of the Ti/Pd@MXene filter was more competitive than that previously reported (0.348 kWh·mmol −1 ), especially for high BrO 3 − removal (≥75 %). This work highlighted an effective flow-through electrocatalytic filter to induce H* -mediated electrochemical reduction of BrO 3 − .
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
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Yuanyuan An,Guoxiu Hao,Xinyue Wang,Li Zhou,Mengyao Wu,Jialong Ma,Lien-Yang Chou
In this study, we synthesized CeO2 possessing an open pore structure and verified its structural differences compared to CeO2 lacking such an open pore structure. Using these two CeO2 samples as catalyst supports and loading them with Pd metals, a series of characterizations were carried out on the resultant catalysts to analyze their structures and properties meticulously. We have elucidated the influence of the open pore structure on the loading position of Pd. Hydrogenation reactions involving alkynes and alkenes were employed to confirm the existence of steric hindrance effects caused by the pore structure differences. Furthermore, we applied these catalysts to more valuable industrial reaction systems, demonstrating that the unique pore structures of directly synthesized CeO2 can also exhibit excellent performance in practical applications.
研究领域:
材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2024
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IF 4.2
Yanhu Li,Mei Chen,Linghong Xue,Xu Li,Qingji Wang
Metal oxide semiconductor (MOS) sensor, one of the most widely used gas sensors, faces significant challenges in achieving lower detection limit. Addressing this issue, the utilization and strategic design of bimetallic catalysts present a promising avenue. In this paper, Pd-Pt was in-situ grown on ZnO nanoflowers directly prepared on planar substrate and a sensor for detecting acetone was developed. The test results reveal that the Pd-Pt/ZnO nanoflowers sensor exhibits a remarkable 107.6 response to 100 ppm acetone at 350 °C, while presenting a rapid response (15s). Moreover, this sensor demonstrates excellent capability in detecting acetone at concentrations as low as 1 ppb, showcasing impressive gas-sensing performance. The response of the sensor to 100 ppm acetone is twice that of ethanol at the same concentration. The exceptional performance of the sensor results from its distinctive nanoflower structure and the catalytic effect of the Pd-Pt, which offers an extensive surface area and enhances the rate of redox reaction for gas molecules. This in-situ grown method has great potential for improving the gas-sensing performance in gas sensor.
研究领域:
材料科学
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化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2017
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IF 3.359
Fuhai Li,Yun Shang,Zuoming Ding,Hanqin Weng,Jiaxin Xiao,Mingzhang Lin
The extraction and separation of platinum group metals (PGMs) from HLLW is of great value for resource recycling and the running of reprocessing plants. In this paper, the photochemical method was proposed to extract and separate PGMs (Pd, Ru) from simulated high level liquid wastes (HLLW). Pd and Ru metal were extracted from aqueous solution by photoreduction with high efficiency (reduction ratio >90%) in the presence of alcohols, which was confirmed by UV–vis spectroscopy, XRD, XPS and TEM analysis. The effects of various parameters such as exposure wavelength, reducing agents, Cl − and pH value were investigated to optimize the photoreaction. The highly efficient extraction and separation of Pd or/and Ru metal from their mixture with lanthanide (Nd) by selective photoreduction was realized. The results suggest that the photochemical method is a promising method for the efficient extraction and separation of PGMs from HLLW.
研究领域:
化学
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核能工程
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Qianqian Li,Hairong Yue,Changjun Liu,Kui Ma,Shan Zhong,Bin Liang,Siyang Tang
Transformation from photocatalytic oxidative dehydrogenation of ethane (PODHE) to photocatalytic dehydrogenation of ethane (PDHE) is an attractive process. A series of Pd/TiO 2 photocatalysts with different Pd loading amount were synthesized by photochemical deposition. And the Pd particle sizes varied from 1 nm to 4 nm. PDHE happened instead of POHDE over Pd particles smaller than 3 nm. The best PDHE performance (H 2 , 799.4; C 2 H 4 , 614.9, in micromoles per gram of catalyst) was obtained over 0.5 wt.% Pd/TiO 2 catalyst. And it was 3 times of it of PODHE over 1 wt.% Pd/TiO 2 . Reducing the Pd particle size of Pd/TiO 2 would increase Pd 0 /Pd 2+ and lower the valence band and conductive band of Pd/TiO 2 , which affect the catalytic behaviors. Detailed formation of products was investigated in this work.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
COLLOID AND POLYMER SCIENCE
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2017
·Vol. 295
·期 4
·703-707
·
IF 1.723
Lu Wangting,Zhang Geng,Wei Feng,Li Wenhui,Cheng Kun,Ding Fei,Zhang Jiying,Zheng Wanquan
Palladium nanocrystals (NCs) are highly useful functional materials in many applications, and the performances of Pd NCs were strongly depended on the crystalline facet exposed on their surface. In this work, Pd NCs were synthesized in aqueous solutions by using Na 2 PdCl 4 as the precursor, citric acid as the capping agent, and Pluronic F127 as both stabilizer and reductant. By adjusting the reaction parameters, Pd cuboctahedrons, octahedrons, and triangular nanoplates with well-defined facets can be produced. This study provides a new pathway for the shape-controlled preparation of noble metal NCs.
研究领域:
材料科学
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化学
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产品关联
DOI
高影响因子
VACUUM
·
2025
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IF 3.9
Xiaohua Wang,Yanwei Li,Xinhui Jin,Guang Sun,Jianliang Cao,Yan Wang
The pressing need for health and environmental protection has sparked significant interest among researchers in exploring gas sensors made from metal oxide semiconductors (MOSs). Herein, a co-modification approach involving palladium (Pd) and palladium oxide (PdO) is introduced to enhance the sensing properties of indium oxide (In 2 O 3 ) to hydrogen sulfide (H 2 S). Pd and PdO co-modified In 2 O 3 hierarchical porous nanocubes (Pd/PdO-In 2 O 3 HPNCs) were synthesized using a facile hydrothermal method. With the theoretical doping amount of 2 mol%, the synergistic effect of metal Pd and PdO-In 2 O 3 heterojunction made Pd/PdO-In 2 O 3 show excellent sensing performance to H 2 S compared to In 2 O 3 . Specifically, the material features a lower operating temperature (280 vs 300 °C), higher sensitivity (95.06 vs 28.59 to 20 ppm H 2 S; 2.28 vs 1.17–100 ppb H 2 S), and better selectivity (7.41 vs 2.32 times to triethylamine), while also demonstrating satisfactory reproducibility and stability. The synergistic sensitization mechanism of noble metal catalysis and heterojunction in Pd/PdO–In 2 O 3 HPNCs, along with their underlying mechanism, was discussed. Integrating noble metal modification with heterojunctions adds complexity to the structure and composition of the material. The synergistic effects of these two sensitization strategies on the H 2 S sensitization mechanism need further in-depth investigation.
研究领域:
材料科学
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化学传感器
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纳米技术
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环境监测
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半导体物理
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Mengyu Li,Wei Zhuang,Xia Meng,Wenxia Zhang,Keke Zhang,Zhenfu Wang
Metal-enzyme integrated catalysts combine the high selectivity of enzyme catalysts with the broad substrate spectrum of metal catalysts and offer tremendous possibilities for chemoenzymatic cascade processes. However, the rational design of microenvironments in nanostructures that make metals and enzymes compatible for efficient activity still remains challenging. In this report, a nanocomposite catalyst was fabricated by integrating ultrafine Pd nanoparticles (Pd NPs) and Candida antarctica lipase B (CALB) on the hydrophobic polydopamine-coated SiO 2 (SP) to enhance the compatibility of enzyme-metal catalysts. In detail, Pd NPs were in situ reduced by PDA on the SP surface, and the obtained SP-loaded Pd (Pd/SP) was hydrophobically modified by octadecyltrimethoxysilane for the subsequent adsorption immobilization of CALB to prepare the integrated catalyst, CALB/mPd/SP. The hydrophobic PDA coating on SiO 2 not only stabilized the loaded ultrasmall Pd nanoparticles but also facilitated the activation of the immobilized lipase, which helped to improve the cascade catalytic efficiency of CALB/mPd/SP. Afterward, CALB/mPd/SP was used in a one-pot dynamic kinetic resolution (DKR) reaction of α-phenylethylamine with high conversion (>99 %), selectivity (93.9 %), and ee p (>99 %). After 25 days of storage and 5 h of sonication, CALB/mPd/SP exhibited no significant reduction in the DKR catalytic activity. This study proposed a simple and sustainable method for the preparation of enzyme-metal cascade catalysts to enhance their stability and achieve significantly increased activity through interfacial microenvironmental modulation.
研究领域:
生物化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
Junjie Zhou,Ning Li,Jialu Shen,Xu Meng,Xiang Liu
Hydrogen has attracted much attention as one of the most promising chemical fuel candidates because of its zero emission during consumption. In order to solve the freezing problem of water based hydrolysis process, herein, the Pd/C as an efficient and stable catalyst for the methanolysis, ethanolysis, propanolysis and butanolysis of B 2 pin 2 for the generation of hydrogen has been first developed. The large kinetic isotope effect (KIE) of k H /k D = 5.0, D 2 formation from CD 3 OD and in situ tandem reaction have confirmed that alcohol is the only hydrogen source. Interestingly, the order of E a of these alcohols in H 2 evolution is MeOH (methanol, 29.57 kJ/mol) < EtOH (ethanol, 34.80 kJ/mol) < PrOH (propanol, 39.08 kJ/mol) < n BuOH (n-butanol, 41.98 kJ/mol), which is consistent with the known order of acidities of these alcohols (MeOH > EtOH > PrOH > n BuOH).
研究领域:
化学
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催化科学
✓ 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）