Materials
·
2026
·Vol. 19
·期 17
·3673
·
IF 3.7
Caimei Ma,Jiangbing Li,Xinlu Fan,Qingyang Yu
Aiming at the problem that the selectivity of heterogeneous catalysts is difficult to be controlled and the active components are easy to be lost in the acetylene double carbonylation reaction, this paper constructs a highly efficient Pd-based catalyst through the combination of carrier morphology engineering and surface basicity regulation. Using melamine/urea as a precursor, tubular carbon nitride (TCN) was constructed by hydrothermal calcination, and then Pd/TCN-series catalysts were prepared by ultrasonic-assisted impregnation loading 5 wt% Pd and heat treatment in a N2atmosphere. At the same time, bulk g-C3N4(BCN) and activated carbon (AC), TiO2, and ZSM-5 supported systems were used as controls. The characterization results show that compared to BCN, TCN-500 (calcined at 500 °C) has a higher specific surface area (40.19 m2/g vs. 12.47 m2/g) and pore volume (0.1850 cm3/g vs. 0.0792 cm3/g), which provides abundant anchoring sites and efficient mass-transfer channels for Pd nanoparticles. After the introduction of Pd, the total base amount of the catalyst increased significantly from 0.4866 to 1.7172 mmol/g, and the strong Lewis-base center was significantly enhanced. TEM/XRD confirmed that Pd was uniformly dispersed on TCN-500 and mainly exposed the (111) crystal plane. XPS further revealed that there was a stronger electron-coupling effect between Pd and the support. Under the reaction conditions of 70 °C and 5 h, the selectivity of Pd/TCN-500 to dimethyl butenedioate was up to 83.7% (acetylene conversion was 59.6%), which was significantly better than that of the contrast carrier system. The cycle test showed that the selectivity and conversion of the catalyst were reduced to 54.4% and 41.1%, respectively, on the third use. The performance degradation was mainly attributed to the oxidative damage of the TCN nanotube skeleton and the passivation of the surface active defect sites. In this study, the synergistic effect of tubular morphology and surface Lewis basicity effectively stabilized the Pd active center and regulated the product selectivity, which provided a new idea for the development of efficient heterogeneous catalysts for acetylene double carbonylation in non-petroleum routes.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Yuqi Zhang,Zetao Mou,Jun Li,Panmei Liu,Yuan Huang,Zumin Wang
The development of high-performance Pd-based composite catalysts is of great significance for the advancement of direct ethylene glycol fuel cells. In this work, we prepared a Pd/Ni x Zn 1- x O-C catalyst for the ethylene glycol oxidation reaction (EGOR). The porous flocculent structure and large specific surface area of Ni x Zn 1- x O provide abundant adsorption sites for Pd nanoparticles, which reduces their sizes and improves their dispersion. In addition, the Ni x Zn 1- x O offers additional active sites for EGOR. The Pd/Ni x Zn 1- x O-C catalyst exhibits excellent EGOR performance. The mass activity of Pd/Ni x Zn 1- x O-C is 6004.0 mA mg −1 Pd , which is 6.3 times higher than that of commercial Pd/C. The structural studies prove the successful construction of hetero-interfaces between Pd and Ni x Zn 1- x O, which effectively modulates the electronic structure of Pd. The excellent catalytic performance is mainly attributed to (i) the synergistic effect between Pd and Ni x Zn 1- x O, (ii) improved utilization efficiency of Pd nanoparticles, and (iii) the large specific surface area of Ni x Zn 1- x O. The work thus provides valuable insights for the development of high-performance Pd-based composite EGOR catalysts.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源材料
·
燃料电池
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Lu Zhang,Guijiu Xie,Fuyi Liu,Huiming Ji
Hydrogen sensors are very important for real-time detection of hydrogen leakage. In this study, a Pd-Ni film hydrogen sensor with high hydrogen response and selectivity was fabricated. A 1.3 µm-thick organosilica membrane was coated on the surface of Pd-Ni alloy film by sol-gel process and hot-coating method to fabricate a 1,2-bis(triethoxysilyl)methane (BTESM)-coated Pd-Ni film hydrogen sensor, which endows the sensor with superior H 2 selectivity due to the molecular sieve property. And the gas sensing performance was tested at optimum operating temperature. The results show higher response is obtained in both N 2 and air atmosphere by hybrid organosilica membrane modification on the Pd-Ni film sensor. Very importantly, the response of the sensor to hydrogen is greatly improved and well maintained in the presence of oxygen, although the response/recovery time increased. The organosilica membrane has high permeability to hydrogen with the kinetic dimater of 0.289 nm while effectively inhibits the permeation of relatively larger gas molecule such as oxygen (0.34 nm) and methanol (0.38 nm), resulting in excellent selectivity to H 2 . The mechanism of response and selectivity enhancement is explored.
研究领域:
材料科学
·
化学工程
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2019
·
IF 3.131
Siwen Xia,Yu Yang,Wenjing Zhu,Changli Lü
Hydrophilic quaternized polyhedral oligomeric silsesquioxane (QPOSS) stabilized palladium nanoparticles hybrids (PdNPs@QPOSS) were successfully constructed for catalytic reduction of organic dyes and nitrophenols. The size of PdNPs can be effectively regulated through the molar ratio between QPOSS and Pd precursors. Uniformly dispersed nano-sized QPOSS encapsulated ultra-fine PdNPs with average diameter of 2.38 nm were obtained as the molar ratio of precursors was 1:8. It was found that low-dose PdNPs@QPOSS nanohybrids as catalysts exhibited outstanding catalytic reduction activity for methylene blue (MB) and nitrophenol (4-NP) with high conversion frequencies (TOF) of 213.7 and 17.8 min −1 respectively, which is superior to commercial Pd/C catalyst. The nanocatalysts we prepared could be stably dispersed in water for one month and there was no significant loss of catalytic activity in four catalytic cycle. The enhanced catalytic activity and good stability can be attributed to QPOSS as a stabilizer having strong coordination with as-generated PdNPs. In addition, we evaluated the decolorizing properties of common organic pollutants including methyl orange (MO), congo red (CR), methyl orange (MO), rhodamine 6G (R6G), rhodamine B (RhB), rhodamine 6G (R6G), and nitrophenol derivatives. The organic-inorganic hybrid nanocatalyst PdNPs@QPOSS is very effective in catalytic reduction of a series of colored dyes and nitrophenols, which also means that the nanohybrid as catalyst has a wide range of applications in industrial degradation of organic pollutants in wastewater.
研究领域:
材料科学
·
催化
·
环境化学
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xue Li,Xue Zhao,Yingtang Zhou,Jiao Hu,Hucai Zhang,Xun Hu,Guangzhi Hu
Ammonia is used extensively as a raw material for fertilizers and industrial production. However, the ammonia yield of the traditional ammonia production process is far from reaching the requirements of industrial applications. Among various methods, electrochemical ammonia synthesis is the most anticipated. Density functional theory (DFT) calculations show that nanoscaled palladium (Pd) decorated on boron–carbon-nitrogen (BCN) support has great catalytic activity towards nitrate electrochemical reduction. We designed and synthesized the BC2N/Pd (both B and N atomic loading more than 20%) electrocatalysts and applied them to electrochemically convert harmful nitrate to high value-added ammonia, which performed an excellent ammonia yield rate of 1730 μg h −1 cm −2 and a high Faraday efficiency of 97.42% in water that containing 250 mM KNO 3 . Isotope labeling experiments proved that ammonia originates from nitrate reduction. At the same time, BC2N/Pd also exhibits splendid stability and durability. The outstanding electrocatalytic activity suggests good prospects in industrial applications, including the purification of ammonia and nitrate wastewater.
研究领域:
材料科学
·
环境科学
·
催化化学
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高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2022
·Vol. 135
·期 3
·1541-1552
·
IF 1.843
Zhang Zhenwei,Ma Xiaoshi,Yue Chuanjun,Wei Xuejiao,Liu Baoliang
Furfuryl ethyl ether (FEE), an important gasoline additive, is synthesized by a one-step reductive etherification of furfural (FF) by Nb 2 O 5 nanowires loaded with Pd as catalysts. Compared with other materials, the catalyst had a suitable synergistic effect between the reductive sites Pd 0 and the acidic sites of Nb 2 O 5 nanowires, effectively improving the yield of FEE. In ethanol, at 453 K and under 1 MPa H 2 pressure, the catalyst 1.0 wt% Pd/Nb 2 O 5 showed excellent catalytic performance in the reductive etherification reaction, and the yield of FEE reached 87.7%, higher than Pd/C whose yield was 81%. This result showed a feasible way to simplify the FEE preparation process, thus reducing production costs.
研究领域:
催化化学
·
绿色化学
·
纳米材料化学
·
能源化工
·
有机合成
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2016
·Vol. 42
·期 6
·6181-6190
·
IF 1.833
Wang Meng-Meng,Liu Shi-Wei,Li Lu,Yu Shi-Tao,Xie Cong-Xia,Song Zhan-Qian
Rosin hydrogenation using polyvinylpyrrolidone (PVP)-stabilized Pd colloidal nanoparticles as catalyst in an aqueous/organic biphasic system was investigated. The influence of preparation methods on the size of Pd nanoparticles for hydrogenation of rosin was marked. Compared with traditional catalysts Pd/C and Raney-Ni, PVP-stabilized Pd colloidal nanoparticles showed excellent catalytic activity and promoted formation of the product tetrahydroabietic acid (THAA). More than 93 % rosin was hydrogenated, and the mass fraction of THAA was 54.2 % when the reaction was carried out at 160 °C for 4 h. It was also found that PVP-stabilized Pd colloidal nanoparticles exhibited good reusability for hydrogenation, with no obvious decrease in catalytic performance when reused six times.
研究领域:
催化化学
·
纳米材料
·
有机合成
·
绿色化学
·
胶体化学
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高影响因子
IONICS
·
2017
·Vol. 23
·期 7
·1861-1869
·
IF 2.062
Suo Yange,Rong Chenbin,Guo Yuxin,Zhang Zhiguo,Hu Guilin,Xu Yousheng,Zhou Xinfa
This work reports the synthesis of a novel carbon-supported Pd-decorated PtCu nanocatalyst for formic acid oxidation. Without using surfactants or polymers, PtCu alloy was firstly prepared through simply co-reduction of Pt and Cu ions using ethylene glycol and sodium citrate as the reducing and stabilizing reagents. Then, Pd was decorated on the surface of PtCu through spontaneous replacement of Cu by Pd. XRD results suggest that the lattice parameters of the PtCu and Pd-decorated PtCu nanoparticles are smaller than that of Pt. TEM images show that all metallic nanoparticles are well dispersed on the carbon surface. The average particle size of the Pd-decorated PtCu nanoparticles is 2.9 nm. Electrochemical analysis suggests that the carbon-supported Pd-decorated PtCu nanocatalyst exhibits an enhanced activity for formic acid oxidation in comparison with the carbon-supported Pt and carbon-supported PtCu, as well as a high stability in acidic medium.
研究领域:
材料科学
·
电化学
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高影响因子
ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Tareque Odoom-Wubah,Zhenzhen Li,Zhou Lin,Tingting Tang,Daohua Sun,Jiale Huang,Qingbiao Li
Bimetallic Pd-Pt nanoflowers (Pd-Pt NFs) of varying sizes (20–60 nm) were synthesized through the concurrent reduction of Pd(NO 3 ) 2 and K 2 PtCl 4 using Cinnamomum camphora ( C. camphora ) leaf extract assisted by ascorbic acid (AA). C.Camphora acted as both a co-reducing agent and a green template in the synthesis protocol providing a fast, simple, green and cost-effective means of producing the Pd-Pt NFs. Characterization techniques such as X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) were used to confirm the Pd-Pt NFs formation. FT-IR analysis showed that biomolecules such as polyphenols and flavonoids were responsible for the reduction while stretching vibration bands from C H, C C , O H, and C O O acted as capping agents. The as-formed Pd-Pt NFs showed excellent performance and stability in the electro-oxidation of ethanol in alkaline media. Electro-catalytic performance increased with Pt content, while addition of Pd increased stability. The PdPt 3 NFs presented the best performance with a mass activity of 1.43 A mg −1 metal , 5.72, 4.93, 2.27, 1.27, 11 and 4.6% higher than the Pd, Pt, Pd 3 Pt, and PdPt NFs, and commercial Pt and Pd-black respectively. However, it was more prone to poisoning, with an I f /I r value of 0.78 compared to 1.37 for Pd 3 Pt NFs.
研究领域:
材料科学
·
环境科学
·
电化学
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Xingzong Dong,Guangye Liu,Zhaoan Chen,Quan Zhang,Yunpeng Xu,Zhongmin Liu
Compared with the rapid deactivation of the Pd/AC catalyst, an eco-friendly Pd-[DBU][Cl]/AC ([DBU][Cl], 1,8-diazabicyclo[ 5.4.0 ]undec-7-ene hydrochloride) catalyst with enhanced stability was synthesized and applied in the hydrochlorination of acetylene. The Pd-20[DBU][Cl]/AC catalyst exhibits 96.7% acetylene conversion and 98.9% selectivity of vinyl chloride within the 24 h evaluation under the conditions of T = 180 °C, GHSV(C 2 H 2 ) = 360 h –1 and V (HCl)/ V (C 2 H 2 ) = 1.2. The enhanced stability of the Pd-[DBU][Cl]/AC catalyst is attributed to the prevention of the reduction of Pd(II) to Pd(0), the inhibition of the formation of coke deposition on the catalyst surface, and the reduction of the loss of Pd species during the reaction. TPD characterization and DFT theoretical simulations confirmed that the PdCl 2 -[DBU][Cl] complex has stronger adsorption of HCl and weaker adsorption of C 2 H 2 and C 2 H 3 Cl compared to PdCl 2 . Furthermore, the catalytic mechanism of acetylene hydrochlorination over the PdCl 2 and PdCl 2 -[DBU][Cl] site was put forward based on theoretical simulations. The good activity and stability of Pd-20[DBU][Cl]/AC in the 60 h lifetime test indicates that it is likely to be a promising alternative to HgCl 2 catalysts.
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RSC Advances
·
2023
·Vol. 13
·期 22
·14980-14990
·
IF 3.9
Xiaoyu Hu,Jinchuan Wang,Shangkun Li,Xuanhao Hu,Rongxing Ye,Linsen Zhou,Peilong Li,Changlun Chen
Extensive research has been devoted to developing metal nanoparticle (NP) doped porous materials with large hydrogen storage capacity and high hydrogen release pressure at ambient temperature. The ultra-sound assisted double-solvent approach (DSA) was applied for sample synthesis. In this study, tiny Pd NPs are confined into the pore space of HKUST-1, affording Pd@HKUST-1-DS with minimizing the aggregation of Pd NPs and subsequently the formation of Pd NPs on the external surface of HKUST-1. The experimental data reveal that the obtained Pd NP doped Pd@HKUST-1-DS possessed an outstanding hydrogen storage capacity of 3.68 wt% (and 1.63 wt%) at 77 K and 0.2 MPa H2 (and 298 K and 18 MPa H2), in comparison with pristine HKUST-1 and impregnated Pd/HKUST-1-IM. It is found that the storage capacity variation is not only ascribed to the different textural properties of materials but is also illustrated by the hydrogen spillover induced by different electron transport from Pd to the pores of MOFs (Pd@HKUST-1-DS > Pd/HKUST-1-IM), based on X-ray photoelectron spectroscopy and temperature desorption spectra. Pd@HKUST-1-DS, featuring high specific surface area, uniform Pd NP dispersion and strong interaction of Pd with hydrogen in the confined pore spaces of the support, displays the high hydrogen storage capacity. This work highlights the influence of spillover caused by Pd electron transport on the hydrogen storage capacity of metal NPs/MOFs, which is governed by both physical and chemical adsorption.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Ruyu Li,Yu Zhao,Tingting Zhang,Zejin Ju,Xianbing Ji,Yanshuai Cui,Longgang Wang,Haiyan Xiao
The development of nanozymes using noble metal nanoparticles to replace natural peroxidase in bio-related detection has been gain great interest. Noble metal nanoparticles with small size have large specific surface area. However, small noble metal nanoparticles tend to aggregate without stabilizer. In this paper, small Pd nanoparticles (3–6 nm) stabilized by bitter gourd polysaccharide (Pd n -BGP NPs) were prepared by using bitter gourd polysaccharide as reducing agent and stabilizing agent. Pd 25 -BGP NPs had peroxidase-like catalytic property. And the catalytic kinetics of Pd 25 -BGP NPs towards substrates conformed to the Michaelis-Menten equation. Furthermore, a method was established to detect H 2 O 2 using Pd 25 -BGP NPs. The linear range and detection limit of this method was 20–320 μM and 2.04 μM, respectively. Finally, Pd 25 -BGP NPs had good biocompatibility when the concentration was less than 80 μg/mL. The prepared Pd nanoparticles with high stability showed their good prospect in H 2 O 2 detection.
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