ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Yunhong Liang,Hao Zhang,Zhaohua Lin,Suqian Ma,Lei Ren,Luquan Ren
As biomimetic actuators that are operable under low voltages, ionic polymer–metal composites (IPMCs) have been proposed as promising candidates in the field of artificial muscles. In this study, a high specific surface area was obtained by directional roughening of a Nafion surface, and high-quality electrodes containing a Pd buffer layer and a Pt layer were deposited on the Nafion matrix via a method of isopropanol-assisted electroless plating, achieving outstanding electromechanical properties. The proposed IPMC exhibits an excellent tip displacement of 36.5 mm and a large blocking force of 2.4 MPa under a low direct current (DC) voltage. Furthermore, the IPMC has an excellent power density (up to 3966 J/m3) and can lift objects that are 20 times its weight, exhibiting great load capacity. More importantly, the imitation of biomimetic actuation behaviors including the opening/closing of petals and wing flapping of bees at a high frequency (21 Hz) has been demonstrated. The fabrication of high-quality Pd/Pt composite electrodes provides significant improvement for IPMC actuators, which is useful for their applications in medical devices and biomimetic robots.
研究领域:
材料科学
·
仿生学
·
生物医学工程
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2015
·Vol. 5
·期 1
·1-9
·
IF 5.578
Wang Liyuan,Feng Feng,Ma Zhanfang
Electrochemical redox-active species play crucial role in electrochemically multiplexed immunoassays. A one-pot method for synthesizing four kinds of new electrochemical redox-active species was reported using HAuCl 4 and Na 2 PdCl 4 as dual oxidating agents and aniline derivatives as monomers. The synthesized polyaniline derivative-Au/Pd composites, namely poly(N-methyl-o-benzenediamine)-Au/Pd, poly(N-phenyl-o-phenylenediamine)-Au/Pd, poly(N-phenyl-p-phenylenediamine)-Au/Pd and poly(3,3’,5,5’-tetramethylbenzidine)-Au/Pd, exhibited electrochemical redox activity at −0.65 V, −0.3 V, 0.12 V and 0.5 V, respectively. Meanwhile, these composites showed high H 2 O 2 electrocatalytic activity because of the presence of Au/Pd. The as-prepared composites were used as electrochemical immunoprobes in simultaneous detection of four tumor biomarkers (carcinoembryonic antigen (CEA), carbohydrate antigen 19-9 (CA199), carbohydrate antigen 72-4 (CA724) and alpha fetoprotein (AFP)). This immunoassay shed light on potential applications in simultaneous gastric cancer (related biomarkers: CEA, CA199, CA724) and liver cancer diagnosis (related biomarkers: CEA, CA199, AFP). The present strategy to the synthesize redox species could be easily extended to other polymers such as polypyrrole derivatives and polythiophene derivatives. This would be of great significance in the electrochemical detection of more analytes.
研究领域:
生物医学工程
·
分析化学
✓ 已验证
DOI
PubMed
高影响因子
Scientific Reports
·
2017
·Vol. 7
·期 1
·1-10
·
IF 4.259
Wang Guojing,Jing Shengchang,Tan Yiwei
Shape control of noble metal (NM) nanocrystals (NCs) is of great importance for improving their electrocatalytic performance. In this report, branched Pd@Rh core@shell NCs that have right square prism-like arms with preferential exposure of Rh {100} facets (denoted as b-Pd@Rh-NCs thereafter) are synthesized and utilized as an electrocatalyst for the hydrazine electrooxidation (HEO) in acidic and alkaline electrolytes. The b-Pd@Rh-NCs are obtained by the heteroepitaxial growth of Rh on the pre-formed branched Pd NCs (denoted as b-Pd-NCs thereafter) core in the presence of poly(vinyl pyrrolidone) (PVP) and bromide ions. A comparative analysis of the voltammetric data for the HEO shows a higher activity on the b-Pd@Rh-NCs exposed with Rh {100} faces than on Rh black, the b-Pd-NCs, and Pd black in acid and alkaline solutions, indicating a structure sensitivity of the reaction. Analysis of the products from the b-Pd@Rh-NCs catalysed HEO reveals a very high hydrazine fuel efficiency, as determined by on-line differential electrochemical mass spectrometry (DEMS).
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2017
·Vol. 7
·期 6
·1415-1422
·
IF 5.773
Zheng Chen,Hongyan Pan,Qian Lin,Xin Zhang,Sheng Xiao,Shun He
Pd core–silica shell catalysts (PdX@SiO2, X = KBr, CTAB, SC) were prepared with and without the addition of three different functional molecules, potassium bromide (KBr), cetyltrimethyl ammonium bromide (CTAB) and sodium citrate dihydrate (SC), by the reverse micelle method, and then characterized by TEM, XRD, EDS, XPS and N2 adsorption/desorption. Results showed that the addition of functional molecules decreased the Pd particle size of the catalysts, and Br− of KBr and CTAB were selectively adsorbed on the surface of Pd particles. Among the prepared catalysts, the catalyst PdKBr@SiO2 had the highest H2O2 selectivity (98%) and productivity (716 mmol gPd−1 h−1). Compared with the catalyst Pd@SiO2 prepared without any additional functional molecules, whose H2O2 selectivity and productivity were 26% and 396 mmol gPd−1 h−1, respectively, the H2O2 selectivity and productivity of the catalyst PdKBr@SiO2 were 277% and 81% higher, respectively, than those of the catalyst Pd@SiO2. The reason for this was that the Br− of KBr can be easily selectively adsorbed on the coordinatively unsaturated sites of the Pd particle surface, which could decrease the energy of the Pd surface and restrain side reactions by inhibiting the O–O bond cleavage of O2 and H2O2. And the catalyst PdKBr@SiO2 has better stability and recyclability than the conventional supported catalyst Pd/SiO2. In contrast, the catalyst PdSC@SiO2 had the lowest H2O2 selectivity (23%) and productivity (395 mmol gPd−1 h−1) because the catalyst PdSC@SiO2 prepared with the functional molecule SC and without Br− had the smallest Pd particle size, which can lead to more coordinatively unsaturated sites and increase side reactions.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Fen Guo,Yiju Li,Baoan Fan,Yi Liu,Lilin Lu,Yang Lei
To achieve high electrochemical surface area (ECSA) and avoid carbon support and binder in the anode catalyst of direct ethanol fuel cell, herein, we design freestanding core–shell nickel@palladium–nickel nanowire arrays (Ni@Pd–Ni NAs) without carbon support and binder for high-efficiency ethanol electro-oxidation. Bare Ni nanowire arrays (Ni NAs) are first prepared using the facile template-assistant electrodeposition method. Subsequently, the Ni@Pd–Ni NAs are formed using one-step solution-based alloying reaction. The optimized Ni@Pd–Ni NA electrode with a high ECSA of 64.4 m2 g–1Pd exhibits excellent electrochemical performance (peak current density: 622 A g–1Pd) and cycling stability for ethanol electro-oxidation. The facilely obtained yet high-efficiency core–shell Ni@Pd–Ni NA electrode is a promising electrocatalyst, which can be utilized for oxygen reduction reaction, urea, hydrazine hydrate, and hydrogen peroxide electro-oxidation, not limited to the ethanol electro-oxidation.
研究领域:
材料科学
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电化学
·
能源转换与存储
✓ 已验证
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Na Ye,Zhao Jiang,Tao Fang
Direct methanol fuel cells (DMFCs) have attracted extensive attention due to clean, efficient characteristics and portable applications. In this work, a series of Pd x Cu y /reduced graphene oxide (rGO) catalysts are assembled and the catalytic performances are investigated for methanol oxidation reaction (MOR) in alkaline media. The intrinsic surface electronic structures of the Pd x Cu y /rGO bimetallic catalysts are also studied to clarify the reaction mechanism. The results reveal that Pd 1.2 Cu 0.2 /rGO exhibits superior catalytic activity (1101.58 A g Pd −1 ), 4.2 and 5.2 times higher than those of the commercial PtRu/C and Pd/C catalysts. CO stripping suggests that the onset potential for CO oxidation on the Pd 1.2 Cu 0.2 /rGO catalyst is lower than those on the commercial PtRu/C and Pd/C catalysts, implying that the anti-CO poisoning ability is enhanced. Combined with the analysis of X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and Raman, the enhanced catalytic activity and anti-CO poisoning ability are attributed to the charge transfer and lattice compression between Pd and Cu, which modify the d-band center and weaken the adsorption of CO. Furthermore, a volcano plot is found between the MOR activity and d-band center, indicating that the excellent MOR activity is attributed to the optimal d-band center with the moderate adsorption strength of CO-like intermediates.
研究领域:
材料科学
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电化学
·
催化反应
✓ 已验证
DOI
高影响因子
ChemistrySelect
·
2022
·Vol. 7
·期 47
·e202203577
·
IF 2.307
Yang Si,Song Liu,Weixing Ming,Wei Wei,Lu Ji,JianJun Zhang,Tingwang An,Dangsheng Gong,Jingnan Zhao,Qingwei Meng,Dongmao Yan
Graphical A continuous flow system are constructed by micropacked-bed reactor and Pd(OH) 2 /C. For the hydrogenation of a series of aromatic dinitro compounds, the continuous flow system demonstrates exceptional performance. Compared with the batch strategy, the continuous flow approach exhibits excellent performance and provides an efficient synthesis technology in hydrogenation of chemicals. Due to the intricacy aromatic dinitro compound hydrogenation processes, it is difficult to attain high conversion and selectivity using merely modified catalysts in batch reactors. The micropacked-bed reactor (μPBR) offers efficient heat and mass transfer, a precise and controllable reaction process, and a high level of safety. In this work, the hydrogenation of 2,4-dinitroanisole was selected as the model reaction, and a variety of catalysts were utilized in the continuous flow system based on μPBR for hydrogenation of 2,4-dinitroanisole. During 960 minutes of operation, the synthesis of 2,4-diaminoanisole was carried out using a Pd (OH) 2 /C catalyst and the optimal process condition, yielding 100 % conversion, 99.5 % selectivity, and the favorable durability. For the hydrogenation of relevant aromatic dinitro compounds, the continuous flow system demonstrates exceptional performance.
研究领域:
化学工程
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催化化学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Qi Ge,Haitao Yu,Li Zhang,Shujing Ni,Wenjin Wu,Han Yang,Jiakang Liu,Kun Huang
In this study, a facile method was developed to synthesize honeycomb-like nitrogen-doped porous carbon nanospheres encapsulated ultrafine Pd nanoparticles (Pd/H-NPCNs) by a combination of one-step Friedel-Crafts reaction between carbazole and benzylamine monomers and subsequent in-situ impregnation-pyrolysis reduction strategy. The obtained Pd/H-NPCNs are further treated with H 2 O 2 to remove carbon layer from the surface of metal to produce Pd/H-NPCNs-H 2 O 2 catalyst. Owing to the high surface area, hierarchically porous structure and special honeycomb-like morphology, the Pd/H-NPCNs-H 2 O 2 catalyst shows the excellent catalytic performance in the selective hydrogenation of cinnamaldehyde (CAL) under mild reaction conditions and water as a green solvent.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Luming Wang,Guoliang Zhang,Hui Zhao,Gang Wang,Zengxi Li,Chunshan Li
Recently, the development of separable and recycling heterogeneous catalyst for ethylene hydroesterification to methyl propionate (MP) has attracted wide interest of researchers. Herein, a kind of 1, 2-bis(di- tert -butyl phosphinomethyl)benzene (dtbpb)-functionalized hypercrosslinked polymers (HCPs) coordinated with Pd single-atom sites was designed and utilized for heterogeneous hydroesterification of ethylene to MP using CO and methanol. The as-prepared catalyst series were characterized with FT-IR, SEM, XPS, NMR, HRTEM, HAADF-STEM, and XAS, which confirmed the coordination structure of Pd with dtbpb ligand linked to HCPs, as well as the dispersion of Pd in the form of single atoms on the polymer support. The effects of Pd loading and reaction conditions on the ethylene hydroesterification were systematically investigated. As a result, 100 % selectivity of MP with 96.2 % conversion of ethylene were achieved on Pd/dtbpb@HCPs catalyst under the optimal condition and no obvious deactivation behavior was observed during the recycling evaluation. The detailed reaction mechanism of ethylene hydroesterification was proposed by identification of crucial intermediates of Pd-H, Pd-alkyl and Pd-acyl species by employing in-situ DRIFTS. The kinetic study was conducted and the reaction orders of ethylene and CO are corresponding to 0 and 0.5, with the activation energy of 50.7 kJ/mol.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Jing Zekun,Guo Yakun,Wang Qi,Yan Xinrong,Yue Guozong,Li Zhendong,Liu Hanwen,Qin Ruixuan,Zhong Changyin,Li Mingzhen,Xu Dingguo,Yao Yunxi,Yao Yonggang,Shuai Maobing
Hydrogenation is a versatile chemical process with significant applications in various industries, including food production, petrochemical refining, pharmaceuticals, and hydrogen carriers/safety. Traditional hydrogenation of aromatics, hindered by the stable π-conjugated phenyl ring structures, typically requires high temperatures and pressures, making ambient hydrogenation a grand challenge. Herein, we introduce a PdPtRuCuNi high entropy alloy (HEA) nanocatalyst, achieving an exceptional 100% hydrogenation of carbon-carbon unsaturated bonds, including alkynyl and phenyl groups, in solid 1,4-bis(phenylethynyl)benzene (DEB) at 25 °C under ≤1 bar H 2 and solventless condition. This results in a threefold higher hydrogen uptake for DEB-contained composites compared to conventional Pd catalysts, which can only hydrogenate the alkynyl groups with a ~ 27% conversion of DEB. Our experimental results, complemented by theoretical calculations, reveal that PdPtRu alloy is highly active and crucial in enabling the hydrogenation of phenyl groups, while all five elements work synergistically to regulate the reaction rate. Remarkably, this newly developed catalyst also achieves nearly 100% reactivity for ambient hydrogenation of a broad range of aromatics, suggesting its universal effectiveness. Our research uncovers a novel material platform and catalyst design principle for efficient and general hydrogenation. The multi-element synergy in HEA also promises unique catalytic behaviors beyond hydrogenation applications.
研究领域:
化学工程
·
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Zhenxing Wang,Hongli Zhao,Kaicha Chen,Hongyuan Li,Minbo Lan
Signal amplification is crucial to improve the sensitivity for the electrochemical detection of cardiac troponin I (cTnI), one of the ideal biomarkers for early acute myocardial infarction (AMI) diagnosis. Herein, we developed a novel signal amplification strategy to construct a sandwich-type electrochemical aptasensor for the detection of cTnI. Core-shell [email protected] dendritic bimetallic nanoparticles loaded on melamine modified hollow mesoporous carbon spheres ( [email protected] DNs/NH 2 -HMCS) was prepared as labels to conjugate with thiol-modification DNA aptamers probe for signal amplification. While introducing numerous amino groups, the melamine functionalized hollow mesoporous carbon spheres (NH 2 -HMCS) retained the edge-plane-like defective sites for the adhesion and electrocatalytic reduction of H 2 O 2 . With the unique characteristics of NH 2 -HMCS, it not only enhanced the dispersity and loading capacity of core-shell [email protected] dendritic bimetallic nanoparticles ( [email protected] DNs), but also improved the stability of bonding by the affinity interaction between [email protected] DNs and amino groups of melamine. Meanwhile, the synergistic catalysis effect between [email protected] DNs and NH 2 -HMCS significantly enhanced the electrocatalytic reduction of H 2 O 2 and further amplified the signal. Under optimal conditions, this recommended aptasensor for cTnI detection displayed a wide dynamic range from 0.1 pg/mL to 100.0 ng/mL and a low detection limit of 15.4 fg/mL (S/N = 3). The sensor also successfully realized the analysis of cTnI-spiked human serum samples, meaning potential applications in AMI diagnosis.
研究领域:
医学诊断
·
纳米材料科学
·
生物传感技术
✓ 已验证
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2019
·
IF 2.781
Xiaofang Wan,Xinying Wang,Guangxue Chen,Congbao Guo,Bowen Zhang
Covalent organic frameworks (COFs) have attracted much attention due to their high porosity and highly ordered crystalline structure. However, the insoluble and unprocessable features of bulk COF powder limit their applications. To overcome these limitations, COF-TpPa film was prepared based on amine-group functionalized nanofibrillated cellulose (NFC) by Schiff base reaction for the first time. The obtained COF-TpPa/NFC membrane had high specific surface area (BET, 357 m 2 /g) and uniform pore size of 2–20 nm with the thickness of 250 nm. Via a simple post-treatment, a Pd-containing Pd@COF/NFC composite membrane , was accordingly synthesized, which showed excellent catalytic activity in catalyzing dechlorination of o -dichlorobenzene ( o -DCB) with high activity (the apparent reaction rate was 0.0235 min −1 ).We expect that our approach will further boost research on designing and employing functional COF film for catalysis.
研究领域:
材料科学
·
环境科学
·
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）