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
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环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2013
·Vol. 69
·期 3
·580-586
·
IF 1.102
Meng Lifen,Cheng Jiaxi,Yang Yaling
A simple and practical extraction method of supramolecular solvents (SUPRAS) was developed for separation and enrichment of trace amounts of palladium (Pd) and silver (Ag) in water samples prior to flame atomic absorption spectrometry (FAAS) analysis. The SUPRAS selected was made up of an aqueous solution containing tetrahydrofuran and nonanoic acid. Pd and Ag reacted with diethyldithiocarbamate to form hydrophobic chelates, which were extracted into the vesicles of SUPRAS. Different parameters such as the concentration of chelating agent, sample pH, supramolecular solvent and the effect of foreign ions were studied. Under the optimal conditions, the linear ranges of Pd and Ag were from 10 to 1,000 μg/L. The relative recoveries of Pd and Ag in tap and river water samples at the spiking level of 10 ug/mL ranged from 90.8 to 116%. The relative standard deviations were 3.6–4.0% ( n = 9), the limits of detection were 2.8 and 1.9 μg/L and the enrichment factors were 36 and 18 for Pd and Ag, respectively. The quantification limits were 3.2 and 2.4 μg/L. The method was successfully applied to the determination of Pd and Ag in water samples.
研究领域:
分析化学
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环境化学
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分离科学
·
痕量元素分析
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样品前处理
✓ 已验证
DOI
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2020
·Vol. 37
·期 4
·614-622
·
IF 2.69
Haleem Abdul,Syaal Sidra Bibi,Ajmal Muhammad,Ambreen Jaweria,Rauf Sajid,Ali Nasir,Muhammad Saz,Shah Afzal,Zia Muhammad Abid,Siddiq Muhammad
Here in, we demonstrate facile fabrication of silver and palladium nanoparticles in dual responsive poly(N-isopropylacrylamide- co -2-Acrylamido-2-methylpropane sulfonic acid) microgel with temperature- and pH-dependent catalytic potential. Palladium-based catalyst showed better catalytic efficiency as compared to silver-based catalyst for degradation of Rhodamine-B and P-Nitrophenol in aqueous medium under the same set of reaction conditions. The responsive nature of the microgel was found to be useful to tune the catalytic activity of the as-prepared catalysts, and reduction rate was enhanced with the pH and temperature elevation of the reaction medium; however, the increasing trend was slowed in the volume phase transition region of the microgel. Under a specific set of reaction conditions, the reduction of Rhodamine-B was as fast as 0.968 and 0.571 min −1 when catalyzed with palladium and silver based catalysts, respectively. The hydrodynamic radius of the particles of microgel support was found to be in the range of 65-180 nm when pH and temperature of the medium were varied in the range of 2-12 and 25-45, respectively. The estimated diameter of silver and palladium nanoparticles fabricated in the microgel support under the same set of reaction conditions was 9-15 and 7-11 nm, respectively.
研究领域:
材料科学
·
化学工程
·
纳米技术
✓ 已验证
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
He Limin,Wang Yangdong,Wang Can,Liu Zhicheng,Xie Zaiku
The hydrogenation of 4-carboxylbenzaldehyde over Pd catalysts is a crucial process during the production of pure terephthalic acid. Herein, ZIF-8 derived carbon materials (NC) with adjustable N types were synthesized and used as the supports of Pd catalysts. Pd supported on NC with 50.5% of pyridinic N exhibited best hydrogenation activity with a TOF value of 4.1 min−1. The microstructures of NC support and electronic structures of Pd in Pd/NC were investigated by techniques such as XRD, N2 physisorption, XPS, H2-O2 titration and TEM. The nitrogen species in CN surface not only can adjust chemical state and dispersion of Pd nanoparticles (NPs), but also promote the adsorption and activation capability of H2 molecular. Besides, the ratio of Pd0/Pd2+ and Pd dispersion were closely correlated with pyridinic nitrogen content. The improvement in hydrogenation activity and stability of Pd/CN catalyst in relative to Pd/C were ascribed to the synergistic effect of pyridinic nitrogen and active site Pd0.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
NANOTECHNOLOGY
·
2018
·Vol. 29
·期 33
·335402
·
IF 3.404
Yiqun Jiang,Man Chen,Yifan Yang,Xuanlin Zhang,Xuezhang Xiao,Xiulin Fan,Chuntao Wang,Lixin Chen
Safe and efficient hydrogen storage is one of the key technologies for the widespread utilization of hydrogen energy. Formic acid (FA) is regarded as a safe and convenient chemical hydrogen storage material. However, the lack of highly efficient heterogeneous catalysts hinders its practical application. Herein, we presented a facile wet-impregnated deposition method to synthesize ultrafine AuPd alloy nanoparticles anchored on TiO2 nanosheets (AuPd/TiO2 nanosheets) which were used as high efficient catalysts for the dehydrogenation of FA. TiO2 nanosheets were calcined at different temperatures to modify the catalytic activity of catalyst. AuPd/TiO2 nanosheets-400 exhibits the superior activity for catalyzing the FA to release 96% of overall hydrogen content with an initial turnover frequency value of 592 mol H2 mol−1 metal h−1 at 25 °C and low activation energy of 11.8 kJ mol−1. Detailed characterizations show that the superior catalytic performance can be ascribed to the alloy structure of AuPd centers, the phase and crystallinity of TiO2 nanosheets, and the strong electron transfer interaction between AuPd nanoparticles and TiO2 nanosheets substrate.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 9
·1130-1137
·
IF 4.568
Ling Shen,Jie Ying,Ge Tian,Mingpu Jia,Xiao-Yu Yang
Graphical A facile solvothermal method is presented to synthesize ultralong PtPd alloyed nanowires anchored on graphene as highly effective MOR catalysts. The rational synthesis of Pt-based alloyed nanowires still remains a great challenge because of the different reduction potentials between Pt and another metal and the intrinsic feature of isotropic growth in face-centered cubic (fcc) structured Pt. In this work, PtPd alloyed nanowires with ultrahigh aspect ratio anchored on graphene (PtPd NWs/graphene) were synthesized by a facile solvothermal method without the use of any templates or surfactants. Due to the integration of ultralong PtPd nanowires and stable graphene support, PtPd NWs/graphene exhibited outstanding electrochemical activity toward methanol oxidation reaction (MOR) in comparison with pure Pt NWs/graphene and commercial Pt/C catalysts. Meanwhile, PtPd NWs/graphene had a much higher current density than Pt NWs/graphene and commercial Pt/C catalysts at a constant potential for 7200s in alkaline methanol solution. Moreover, after 1000 cycles of durability testing, PtPd NWs/graphene retained 89.2% of its initial mass activity, much superior to the 63.7% retained for commercial Pt/C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Chemistry-An Asian Journal
·
2018
·Vol. 13
·期 18
·2708-2713
·
IF 3.692
Haiwen Yu,Siqi Xu,Yijiang Liu,Hongbiao Chen,Huaming Li
Graphical Top of the POPs : A porous organic poly(triphenylimidazole) was loaded with ultrafine palladium nanoparticles and the resultant catalyst (Pd@PTPI-Me) exhibited superior catalytic activity and recyclability for the cyanation of aryl iodides. A new porous organic poly(triphenylimidazole), PTPI-Me, was prepared through a Yamamoto self-coupling reaction of 2,4,5-tris-(4-bromophenyl)-1-methyl-1 H -imidazole (TPI-Me) in the presence of bis(1,5-cyclooctadiene)nickel(0). The polymer was subsequently decorated with Pd nanoparticles (NPs) to afford a heterogeneous cyanation catalyst, Pd@PTPI-Me. Pd NPs with an average diameter of 2.7 nm were grown within the PTPI-Me framework, owing to the coordination of the imidazole rings to the Pd species. The resultant Pd@PTPI-Me catalyst, with a Pd loading of 0.13 mmol g −1 , exhibited superior catalytic activity for the cyanation of aryl iodides. More importantly, the heterogeneous catalyst was also readily recycled and displayed negligible deactivation after five cycles.
研究领域:
材料化学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMISTRY
·
2021
·Vol. 39
·期 10
·2745-2754
·
IF 6
Yinbing Tian,Zijie Tang,Yu Ru,Yuanyuan Wang,Liyi Dai
Main observation and conclusion Three diamines (1,8-diaminooctane/ p -phenylenediamine/biphenylenediamine) with different alkyl groups were used to synthesize the functionalized graphene networks. Pd as the common metal catalyst was used to explore the effects of alkyl types of diamines on anti-stacking, metal anchoring ability of functional graphene and hence the catalytic performance. The results were discussed by characterization of the material and its catalytic properties. All catalysts showed excellent catalytic performance on the Suzuki cross-coupling reaction with a high yield of up to 100%. The p -phenylenediamine and biphenylenediamine functionalized graphene with larger specific surface area was beneficial to improve the stability of the graphene catalyst and maintain good catalytic activity after 5 cycles. The Pd nanoparticles in 1,8-octanediamine materials have smaller size and a smaller loading with the same or even better catalytic performance than p -phenylenediamine, biphenylenediamine materials, due to the stronger electron donating ability of N of octanediamine than that of p -phenylenediamine.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2015
·
IF 4.504
Li-Li He,Pei Song,Jiu-Ju Feng,Wen-Hua Huang,Qiao-Li Wang,Ai-Jun Wang
Bimetallic PdAu alloyed nanochain networks (PdAu NCNs) were facilely prepared by a simple wet-chemical method with the assistance of allantoin as the structure-directing agent and stabilizing agent. Allantoin played an important role in the formation of chain-like networks. The products were mainly characterized by transmission electron microscopy (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy. The as-prepared PdAu NCNs had enlarged electrochemical active surface area, and displayed enhanced electrocatalytic activity toward oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR), showing higher resistance to poisoning CO-like intermediates in MOR and more positive onset potential in ORR as compared to commercial Pd black catalyst. This approach provides a promising route for large-scale preparation of desirable bimetallic catalysts with the assistance of small biomolecules.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qiaoyi Zhang,Hongtan Cai,Xin Liu,Yulin Li,Meiyan Wang,Ge Gao,Zeshuo Meng,Haoteng Sun,Xiufeng Hao
A promising approach for powering hydrogen fuel cells (HFCs) involves the in-situ production of hydrogen from formic acid decomposition, with Pd-based catalysts recognized as effective for formic acid dehydrogenation. However, the immobilization of ultrafine palladium nanoparticles (Pd NPs) on catalytic supports presents a challenge and necessitates further investigation into their formation mechanism. We propose a coordination-induced strategy to understand the behavior of ultrafine Pd NPs formation based on multi-functional groups. To establish the structure–activity relationship for tunable Pd microenvironment and catalytic performance, we synthesized various polyacrylonitrile (PAN) carriers through hydrolysis and amidation modification. Molecular dynamics simulations confirmed that a stronger coordination-induced microenvironment facilitates the dispersion of Pd 2+ , suppressing aggregation and enhancing Pd loading. Our experimental results and density functional theory (DFT) calculations demonstrated that the catalytic activity of Pd@APAN(15_1%) with ultrafine Pd NPs (1.5 nm) exhibits over 10 times higher than that of Pd@PAN NPs with the turnover of frequency climbing from 112.6 h −1 to 1309.4 h −1 at 323 K. And Pd-imine and Pd-secondary amine moieties were verified to contribute to the creation of a favorable catalysis microenvironment. This study provides new insights into the design of modified supports with various groups to load well-dispersed and ultrafine Pd for highly efficient catalysts based on a coordination-induced strategy.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Jian Wang,Yan Zhang,Yang Xu,Peiping Zhang,Qian Gao,Qing Liang,Wei Zhang,Wenqing Li,Ruifeng Guo,Bo Jin,Shiding Miao
The liquid-phase oxidation benzyl alcohol using hydrogen peroxide (H2O2) as an oxidant is a promising and green strategy for manufacturing aldehydes or/and ketones. Herein palladium (Pd) nanoparticles were impregnated in lumens of halloysite nanotubes by using ionic liquid (1-(2′-hydroxylethyl)-2,3-dimethylimidazolium chloride) as directing agents. On the basis of the asymmetric scroll-like structure of halloysite and the catalytic decomposition ability of Pd toward H2O2, the prepared catalyst (Pd-IL-HNTs) exhibited powerful self-propelled movement at an average speed of 276 ± 35 μm/s in 30.0 wt % H2O2 solution. The specific interaction between nanomotors and benzyl alcohol was observed as a consequence of self-moving behavior and hydrophobic interaction introduced by ionic liquid. With the synergistic coupling of the catalytic ability and powerful movement, Pd-IL-HNTs displayed outstanding catalytic benzyl alcohol oxidation performance. Compared to other nonpropelling catalysts using lamellar clay (montmorillonite and kaolinite) as supports, such HNT-based nanomotors registered superior catalytic performance, and the TOF value of 118.1 h−1 was obtained.
研究领域:
化学工程
·
催化科学
·
纳米技术
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2019
·Vol. 12
·期 5
·1376-1384
·
IF 4.495
Wen-Di Guo,Lei Liu,Shu-Qing Yang,Xiao-Chao Chen,Yong Lu,Giang VO-Thanh,Ye Liu
Graphical Synergetic catalysis : The one-pot tandem bis-alkoxycarbonylation of alkynes was accomplished over the bi-functional catalytic system containing Xantphos-modified Pd-complex and Lewis super-acid of Al(OTf) 3 . Via the synergetic catalysis, the involved Xantphos-modified Pd-complex was responsible for the activation of CO and the alkynes through coordination to Pd-center while Al(OTf) 3 was in charge of the activation of the alcohol to facilitate the formation of [Pd−H] + active species. Tandem bis-alkoxycarbonylation of alkynes allows for the preparation of 2-substituted succinates from alkynes and nucleophile alcohol via two successive alkoxycarbonylation with advantages of 100 % atomic economy and simplified one-pot operation. Herein, the one-pot tandem bis-alkoxycarbonylation of alkynes was accomplished over the bi-functional catalytic system containing Xantphos-modified Pd-complex and Lewis super-acid of Al(OTf) 3 . It was found that, via the synergetic catalysis, the involved Xantphos-modified Pd-complex was responsible for the activation of CO and the alkynes through coordination to Pd-center while Al(OTf) 3 was in charge of the activation of the alcohol to facilitate the formation of [Pd−H] + active species. The in situ high-pressure FT-IR analysis, coupled with 1 H/ 13 C NMR spectral characterizations, confirmed that the introduced Al(OTf) 3 with intensive oxophilicity (via acid-base pair interaction) was able to activate nucleophilic MeOH to be a reliable proton-donor ( i. e . hydride-source) to warrant the formation and stability of [Pd−H] + species upon the oxidation of Pd 0 by H + (Pd 0 +H + →[Pd II −H] + ). Over the developed bi-functional catalytic system, the yields of the target diesters were obtained in the range of 36∼86 % in this sequence with the wide substrate scope.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）