ENERGY
·
2025
·
IF 9.4
Xiaohua Li,Zhitao Lei,Yu Cao,Shanshan Shao,Shiliang Wu
The cycloketones were prepared efficiently via the selectively hydrogenation of aqueous phase lignin-derived single phenolic monomer and mixtures. The yield and selectivity of cycloketones was greatly improved over Br modified metal-acid mixed catalyst (PdH5@Br). First, the effect of side-chain functional structures on the aqueous-phase hydrogenation of phenols with Pd/C catalysis was investigated and it was found that the benzene ring with methyl group attached is more easily hydrogenated, and the phenolic hydroxyl side chain was more susceptible to form carbonyl than methoxy groups. A large number of enols existed, thus the catalyst acidity was adjusted by extra addition of HZSM-5, over which the yield of cycloketones from guaiacol was significantly boosted to 67.9%. Subsequently, the electronic properties of catalyst were altered by adding Br over Pd catalyst, weakening the over-chemisorption of intermediate phenol, and the hydrogenating of phenol under PdH5 were enhanced, thus an increased yield of cycloketone of 18.4% occurred. After the hydrotreating of guiaiacol for 2 h at 523 K and 2 MPa H 2 , the yield of cycloketone reached 80.4% on PdH5@Br. The hydrotreating performance of PdH5@Br with lignin-derived phenolic monomer mixtures as the feedstock was also tested, and it presented great universality and stability. It provides an efficient catalyst system and promising technological ideas for biomass hydrotreating.
研究领域:
化学工程
·
可再生资源转化
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产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2024
·
IF 5.2
Yi Wang,Xiaolin Luo,Rui Lu,Fang Lu
Herein, a sustainable route to novel aromatic monomer, dimethyl 1,2,3,4-tetrahydro-1,4-methanonaphthalene-5,8-dicarboxylate, was developed, in which dimethyl muconate and norbornene used as the diene and dienophile undergo Diels-Alder reaction followed by dehydrogenation. The polycyclic cycloadduct, octahydro-1,4-methanonaphthalene-5,8-dicarboxylate, could be synthesized without catalyst. The activated carbon modified with sulfuric acid generated more oxygen-containing groups, stronger acidity and more acidic sites. Highly dispersed palladium metal particles with an average particle size of about 1.0 nm exhibited excellent activity in the dehydrogenation reaction and the yield of target product reached 73.8 %.
研究领域:
化学工程
·
催化材料
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Jialu Huang,Chengwei Deng,Yue Liu,Tingting Han,Feng Ji,Yuehua Zhang,Hongbin Lu,Ping Hua,Bowei Zhang,Tao Qian,Xiaolei Yuan,Yaoyue Yang,Yong Yao
Palladium (Pd) is supposed to be one of the most promising catalytic metals towards ethanol (C 2 H 5 OH) oxidation reaction (EOR). However, Pd electrocatalysts easily suffer from the poisoning of the intermediates (especially CO), resulting in the quick decay of EOR catalysis. Herein, inspired by the Brønsted-Lowry acid-base theory, a “attraction–repulsion” concept is proposed to guide the surface structure engineering toward EOR catalysts. Specifically, we induce Bi(OH) 3 species as Brønsted base onto PdBi nanoplates to effectively repel the adsorption of CO intermediates. The PdBi-Bi(OH) 3 nanoplates show an impressive mass activity of 4.46 A mg Pd -1 during the EOR catalysis and keep excellent stability. Both the stability and enhanced performance are attributed by the interfacial Brønsted base Bi(OH) 3 which can selectively attract and repel reactants and intermediates, as evidenced from in situ measurements and theoretical views.
研究领域:
材料科学
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电化学
·
催化作用
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产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2021
·
IF 4.126
Hanxue Yan,Wenbo Gao,Qianru Wang,Yeqin Guan,Sheng Feng,Han Wu,Qing Guo,Hujun Cao,Jianping Guo,Ping Chen
Palladium (Pd) has long been known to be inactive for dinitrogen activation and hence has received little attention for ammonia synthesis. Herein, we report that the reactivity of Pd is changed when reacting with lithium hydride (LiH) forming a series of lithium palladium hydrides such as LiPdH0.7 and Li2PdH2 (denoted as [Li–Pd–H]). LiPdH0.7 promotes N2 fixation by LiH forming Li2NH and LiPd, and the subsequent hydrogenation of Li2NH and LiPd leads to ammonia and regeneration of LiH and [Li–Pd–H]. Based on these experimental results, an ammonia loop mediated by a [Li–Pd–H]–LiH and LiPd–Li2NH composite pair is proposed and demonstrated. An ammonia production rate of 693 μmolNH3 g–1 h–1 was achieved at 300 °C and 1 bar, which is ca. 7 times that of the neat LiH/Li2NH pair at 350 °C and 1 bar and 2 times that of the thermocatalytic process catalyzed by Ru/MgO at 300 °C and 10 bar.
研究领域:
化学
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催化
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Longqiao Ran,Yongming Sui,Wenhui Wang,Fuxin Wang,Dezhou Zheng,Qi Feng,Ruijing Fu,Guangxia Wang
Direct ethanol fuel cells (DEFCs) provide a portable and environmentally friendly power source with high energy density. However, the slow kinetic of the ethanol oxidation reaction (EOR) has hindered the commercialization of DEFCs. Palladium (Pd)-based nanomaterials are the best promising catalysts for EOR due to the high catalytic activities and relatively abundant reserves. In this paper, we developed a simple and green way for the preparation of palladium hydride (PdH 0.43 ) and Au/PdH 0.43 heterostructures. Ethylene glycol (EG) provided the source of H atoms for the formation of PdH 0.43 in synthesis process. The as-synthesized PdH 0.43 and Au/PdH 0.43 nanocrystals were extremely stable under ambient conditions and annealing at 300 °C under Ar. Compared with PdH 0.43 and commercial Pd/C, Au/PdH 0.43 presented a higher mass activity of 2659 mA mg −1 , a lower oxidation peak potential, and a higher catalytic stability for oxidizing ethanol. Remarkably, the improved catalytic performance might arise from the synergistically modulation of electronic structure, the enhanced resistance to poisoning products and the acceleration of electron transfer by the formation of palladium hydrides and abundant heterostructures of Au/PdH 0.43 . This work provides a promising reference for the development of metal-hydride nanomaterials and heterostructures as efficient catalysts.
研究领域:
材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Jin Wang,Peina Zhang,Yujiao Xiahou,Dayang Wang,Haibing Xia,Helmuth Möhwald
The present work introduces a new way to prepare Au–Pd alloy nanowire networks (NWNs) via deposition of Pd atoms onto Au nanowires in reaction media at room temperature without the aid of additional reducing agents. Thanks to their excellent colloidal stability in water as well as in ethanol, the resulting NWNs can be utilized to produce composite thin films with Nafion (perfluorinated sulfonic acid) with dimensions above dozens of square centimeters by means of solution casting on the glass substrate. Most importantly, these films can be easily transferred onto different solid substrates by lift-off technology. Moreover, the resulting Au–Pd alloy NWNs can also be easily and thoroughly loaded into macroscopic carbon fiber cloth (CFC). Both the Au–Pd alloy NWN/Nafion composite film and the Au–Pd alloy NWN-loaded CFC can be used as flexible electrodes for electrocatalysis of ethanol oxidation, with electrocatalytic performance at different distorted states superior by 2 orders of magnitude to those reported in the literature (e.g., commercial Pd/C catalysts and Pd-based nanostructured catalysts). This work opens new possibilities for the large-scale manufacturing of electrodes for fuel cells.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Qiqi Lu,Xiu-Zhi Wei,Haiyong Wang,Qi zhang,Xinghua Zhang,Lungang Chen,Jianguo Liu,Longlong Ma
The selective hydrogenation of nitrile represents an atom-economical and reliable method to synthesize primary amine, a privileged compound in chemistry, biology, and medicine. However, this approach often displays severe selectivity issues, and additives or reducing agents are generally required to solve this problem. In this work, we aim to synthesize primary amine on a green catalytic system and probe into the catalytic mechanism of Pd-Ni interaction using benzonitrile (BN) as a model compound. The nitrile hydrogenation reaction was catalyzed by bimetallic Pd-Ni oxide nanospecies confined in Silicalite‑1 (S-1) zeolite using H 2 as hydrogen donor without any additive which was environmentally friendly and economic. A 92% yield of benzylamine (BA) was achieved on the [email protected] catalyst with a turnover number (TON) of 1667, and such BA yield was still maintained in upscaling experiment. Detailed characterizations shed light on the mechanism of the extraordinary performance of Pd-Ni oxide nanospecies on base-free nitrile hydrogenation.
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
Catalysis Science & Technology
·
2015
·Vol. 6
·期 9
·3027-3037
·
IF 5.426
Yanan Liu,Yufei He,Daran Zhou,Junting Feng,Dianqing Li
Aiming at the preparation of catalysts with well-controlled structures, bimetallic PdCu catalysts containing only small amounts of Pd were prepared by two different methods for partial hydrogenation of acetylene. The highly dispersed and stable PdCu catalyst with the Pd : Cu atomic ratio of 1 : 40 was obtained from a Pd(OH)2/CuMgAl hydrotalcite (HT) precursor by a modified co-precipitation method. The obtained PdCu catalyst possessed uniform PdCu nanoalloys with an average size of 1.8 ± 0.3 nm. As a comparison, the impregnation method was also employed to prepare bimetallic PdCu catalysts and it was confirmed that the Pd-rich(core)–Cu-rich(shell) structure was dominant. Under identical reaction conditions, approximately 100% conversion and 82% selectivity at 100 °C were achieved using the PdCu nanoalloy catalyst which were 23% and 12% higher than those of the Pd-rich(core)–Cu-rich(shell) catalyst. The preferable activity was ascribed to the homogeneous nanoalloy structure and small size effect. The enhanced selectivity was attributed to the strong synergistic effect of PdCu. More significantly, this superior catalytic performance can be retained after 48 h of continuous reaction due to the excellent resistibility against carbon deposition and the confinement effect.
研究领域:
催化化学
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材料科学
·
有机合成
✓ 已验证
DOI
高影响因子
Green Chemical Engineering
·
2022
·
IF 0
Qing Zeng,Shaonan Tian,Yu Zhang,Hui Liu,Dong Chen,Xinlong Tian,Chaoquan Hu,Jun Yang
Recycling precious metals with high-efficiency is undoubtedly beneficial to optimize resource utilization for environmental remediation and sustainable development. Herein, we report an efficient route to recycle the palladium (Pd) and platinum (Pt) electrocatalysts using a phase transfer method. This strategy involves acidic dissolution of deactivated precious metal (Pd/Pt) electrocatalysts from their loading substrates, mixing with an ethanolic solution of dodecylamine (DDA), subsequent extraction of metal ions into a non-polar organic phase, and final reduction by sodium borohydride to reproduce high-performance electrocatalysts towards typical electrochemical reactions, e.g. , oxygen reduction reaction (ORR) and ethanol oxidation reaction (EOR). In specific, the transfer efficiencies are up to 98% and the final recovery rate is over 85% for Pd and Pt electrocatalysts in each cycle. This approach symbolizes a facile and efficient way to recover precious metals, which might be applied to recycling a wide range of metals in various realms after appropriate modifications.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
DOI
Journal of Saudi Chemical Society
·
2019
·
IF 2.759
Pengwei Gao,Yongmei Xiao,Zhenhua Dong,Hongguo Pan,Wentao Wang
By using urea linked porous organic polymers as template, a new nano palladium catalyst with low Pd loading can be easily prepared (1.0 wt% Pd only). Although such less amount of Pd was contained in this new catalyst, it is still an effective catalyst for the Suzuki-Miyaura coupling of aryl iodines and aryl boric acids, affording biphenyl products in excellent yields with outstandingly enhanced turnover numbers (up to 10,536) under green solvent (water).
研究领域:
催化
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材料科学
·
有机化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Yuan Zhou,Xun Zhu,Biao Zhang,Ding-Ding Ye,Rong Chen,Qiang Liao
Formic acid as a renewable fuel can be converted to clean electricity in fuel cells by high-efficient electrochemical oxidation . The conversion rate is fundamentally dictated by the synergy of interactive aspects: catalytic activity , accessibility to active sites, electron transfer , and anti-poisoning stability. For the first time, ordered mesoporous carbon (OMC) is used as the substrate for Pd–PdO catalyst for fuel cells. The unique ordered pore-channel network of OMC can enhance the spatial dispersion of Pd nanoparticles on the pore-channel wall, while the hollow pore-channel can facilitate reactant transport. Microwave and annealing treatments are found to enhance the chemical reduction and to strengthen the anchoring of Pd–PdO catalyst on OMC substrate, respectively. The OMC supported Pd–PdO catalyst (Pd–PdO/OMC) shows 1.7-fold and an order of magnitude higher mass activity and stability as compared to commercial Pd/C catalyst. For fuel cell testing, the Pd–PdO/OMC catalyst is applied to an air-breathing microfluidic fuel cell and achieves a maximum power density of 63.0 mW cm −2 , at least one-fold higher than similar previous reports.
研究领域:
材料科学
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能源科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ANALYST
·
2021
·Vol. 146
·期 5
·1760-1771
·
IF 4.616
Tao Jiang,Feng Jiang,Zemin Zhuo,Huaxin Liu,Bin Hu,Mei Li,Lei Li,Zhengxu Huang,Zhen Zhou,Zhiqiang Zhu
Inert metals are of much importance and play a key role in modern industrial manufacturing. The analytical techniques of inert metals remain challenging. In particular, the mass spectrometry of inert metal elements is yet to be further developed, which also limits the contemporary conceptual in situ analysis of inert metals. As the representative element, the mass spectral detection of palladium is critical and of far-reaching significance. Herein, we developed a mass spectrometry method, which can be used for the high-speed and in situ analysis of palladium, and even for other inert metals. Combining the line ion trap mass spectrometer with the versatile ambient ionization source, a novel kilowatt microwave plasma torch (MPT) can be used to obtain the fully characteristic MPT mass spectra of palladium. Detailed multistage tandem mass spectra show that the general form of target ions is [M(O2)x(NO)mNy(NO2)n]− for the negative ion mode and [M(H2O)x(NO2)y(N2)m]+ for the positive ion mode. Moreover, the formation and evolution of these palladium complex ions were reasonably derived based on the analysis of MPT background mass spectra. This mass spectrometric technique is also suitable for the determination of the palladium-containing solution in the sub-trace level. Semi-quantitative results showed that the detecting ability for palladium in the negative mode is better than that of the positive mode. Under the negative ion mode, the limit of detection (LOD) for m/z 259 were evaluated to be 0.5 μg L−1 under the optimized conditions of the negative mode, with the linear range of 1–100 μg·L−1 (R2 ≥ 0.9985) and the relative standard deviation (RSD, n = 11) being in the range of 1.20%–5.98% (refer to Table S3). Our experimental data showed that MPT-MS was a promising technique for providing another alternative in the on-site analysis of liquid samples and other intimate relevant fields, as the supplement of ICP-MS for the detection of inert metal elements. On the other hand, this work will also certainly promote the more broad applications of platinum-group elements (PGE) in modern science and industry.
研究领域:
分析化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）