LANGMUIR
·
2015
·
IF 4.457
Zhihai Cao,Hangnan Chen,Shudi Zhu,Wenwen Zhang,Xufang Wu,Guorong Shan,Ulrich Ziener,Dongming Qi
Janus Pd/SiO2 nanocomposite particles (NCPs) were successfully synthesized through a combination of the sol–gel process of tetramethoxysilane in inverse miniemulsions and in situ reduction of Pd salts via a gas diffusion process of hydrazine. The formation of Pd nanoparticles (NPs) was verified by X-ray diffraction. The Janus morphology of the Pd/SiO2 NCPs was confirmed by microscopic observation. The Pd/SiO2 NCPs displayed a mesoporous structure. The content of Pd NPs in the NCPs could be conveniently adjusted by the K2PdCl4 loading. A formation mechanism of the Janus Pd/SiO2 NCPs was proposed. The mesoporous Janus Pd/SiO2 NCPs show good catalytic activity toward the reduction of p-nitrophenol with NaBH4.
研究领域:
材料科学
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纳米技术
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催化化学
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胶体与界面化学
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Kaifeng Wang,Song Shu,Min Chen,Junxi Li,Kai Zhou,Jian Pan,Xialing Wang,Xiangjun Li,Jianping Sheng,Fan Dong,Guangming Jiang
Electrocatalytic hydrodechlorination (EHDC) provides one promising solution to mitigate challenges from the water pollutions by persistent chlorinated organics. Palladium (Pd) has shown appealing properties as EHDC catalysts, while the low earth abundance has urged us to raise its activity and minimize usage. Herein, one novel semiconductor-metal Pd-TiO 2 Schottky heterojunction catalyst was developed, which notably outperformed the conventional Pd-C catalyst in mass activity, dechlorination degree and energy selectivity towards EHDC of 2,4-dichlorophenol (2,4-DCP) in water. A combined experimental and DFT calculation study on mechanism revealed that the primary product phenol had a considerable negative effect on EHDC by competing the active sites with 2,4-DCP. The enhanced performance of Pd-TiO 2 originated from the Schottky heterojunction-induced metal-support interactions, which optimized the Pd electronic structure and balanced the 2,4-DCP adsorption and phenol desorption on Pd. This study highlights one novel strategy to boost the metal performance in electrocatalytic hydrogenation reactions.
研究领域:
环境科学
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材料科学
·
催化化学
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DOI
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Lan-Ying Liu,Guo-Shuai Liu,Shi-Ming Niu,He Liu,Min-Hua Cui,Ai-Jie Wang
In this study, a Pd@MXene catalyst was synthesized to enhance the electrocatalytic hydrodehalogenation (ECH) of emerging halogenated organic pollutants (HOPs) by improving the dispersibility, catalytic activity , and stability of palladium (Pd). The average size of Pd nanoparticles (NPs) was reduced to 3.62 ± 0.34 nm with a more intensive peak of Pd (111), which facilitated atomic hydrogen (H*) production. The Pd@MX/CC electrode demonstrated superior ECH activity for diclofenac (DCF) degradation, with a reaction rate constant ( k obs ) 2.48 times higher than that of Pd/CC (without MXene). The satisfactory ECH performance of Pd@MX/CC remained consistent within a wide range of initial DCF concentrations (5–100 mg/L), and no significant ECH attenuation was observed even after up to 10 batches. Furthermore, the high activity of Pd@MX/CC was also observed in the ECH of other halogenated organic pollutants (levofloxacin, tetrabromobisphenol A, and diatrizoate). Density functional theory (DFT) calculations revealed that electronic configuration modulation of the Pd@MXene catalyst optimized binging energies to H* , DCF, and dechlorinated products, thereby enhancing the ECH efficiency of DCF.
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高影响因子
Journal of the American Chemical Society
·
2023
·
IF 15
Xuan Huang,Bingyan Xu,Jie Feng,Shengnan Hu,Wenjie Dou,Tang Yang,Changhong Zhan,Shangheng Liu,Yujin Ji,Youyong Li,Chih-Wen Pao,Zhiwei Hu,Qi Shao,Xiaoqing Huang
Phase regulation of noble metal-based nanomaterials provides a promising strategy for boosting the catalytic performance. However, realizing the continuous phase modulation in two-dimensional structures and unveiling the relevant structure-performance relationship remain significant challenges. In this work, we present the first example of continuous phase modulation in a library of Pd–Te hexagonal nanoplates (HNPs) from cubic-phase Pd4Te, rhombohedral-phase Pd20Te7, rhombohedral-phase Pd8Te3, and hexagonal-phase PdTe to hexagonal-phase PdTe2. Notably, the continuous phase regulation of the well-defined Pd–Te HNPs enables the successful modulation of the distance between adjacent Pd active sites, triggering an exciting way for tuning the relevant catalytic reactions intrinsically. The proof-of-concept oxygen reduction reaction (ORR) experiment shows a Pd–Pd distance-dependent ORR performance, where the hexagonal-phase PdTe HNPs present the best electrochemical performance in ORR (mass activity and specific activity of 1.02 A mg–1Pd and 1.83 mA cm–2Pd at 0.9 V vs RHE). Theoretical investigation reveals that the increased Pd–Pd distance relates to the weak *OH adsorption over Pd–Te HNPs, thus contributing to the remarkable ORR activity of PdTe HNPs. This work advances the phase-controlled synthesis of noble metal-based nanostructures, which gives huge impetus to the design of high-efficiency nanomaterials for diverse applications.
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PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2013
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IF 1.304
Ying Liu,Yangcheng Lü,Guangsheng Luo
A phosphine-functionalized polystyrene microcapsule with hundreds of microns in size was prepared using a microfluidic platform. The size distribution was narrow and the average size could be adjusted in the range 300-400 μm. The morphology and composition of the microcapsules were characterized using scanning electron microscopy, energy-dispersive X-ray spectroscopy, and inductively coupled plasma atomic emission spectroscopy. The results verified the effectiveness of the strategy we proposed for preparing uniform microcapsules with stable Pd immobilization. A Suzuki coupling reaction between aryl halides and phenylboronic acid was used as the model to evaluate their catalytic activity after Pd(PPh 3 ) 4 immobilized onto the microcapsule. It was found that the catalytic activity of microcapsule-supported Pd was always higher than that of the corresponding homogeneous catalyst, and was similar with that of the literature reported microcapsule-supported catalyst with about 7-8 μm particle size. Microcapsule-supported Pd with microcapsules of hundreds of microns in size, being easy to recover, showed good reusability and undetected active species loss, its productivity effect and controllability of the microcapsule-supported Pd catalyst were also expected to benefit from continuous preparation using the microfluidic platform. Moreover, they could be potentially exploited in a fixed-bed reactor with high catalyst density and good mechanical stability.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Hongyu Yang,Zhenghua Tang,Wei Yan,Likai Wang,Qiannan Wang,Yongqing Zhang,Zhen Liu,Shaowei Chen
Peptide-capped nanoparticles represent a unique type of nanomaterials with emergent optical and electrochemical properties . Herein, a series of peptide capped palladium nanoparticles have been prepared and employed as highly efficient catalysts for oxygen electroreduction. The peptide sequence was tuned by substituting amino acid residues at specialized positions, and strong surface effects were observed between the peptide sequence and the electrocatalytic activity. The findings corresponded well with the previously reported C C coupling catalytic reactions, indicating that the residue-specific binding effects but not the overall binding strength governed the electrocatalytic activity. The results may shed light on the rational design of bio-inspired nanomaterials with optimized electrocatalytic properties.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Fangxu Lu,Song Wen,Jie Jiang,Jinchong Zhao,Changsheng Zhang,Junjie Feng,Jing Zhang,Bing Sun,Wei Xu
It is generally acknowledged that the crystal structure of the support plays a crucial role in the catalytic performance, however, the exact role of crystal structure in the catalytic system remains controversial. The Pd/TiO2 catalysts designed in this study with different crystals (rutile (r) and anatase (a)) were employed to study the effects of the crystal structure via a probe reaction for oxygen removal under a hydrogen atmosphere. Under the same reaction conditions, the temperature to achieve 90% O2 conversion on Pd/a-TiO2 could reach up to 150 °C, which is ∼1.4 times (107 °C) that of the Pd/r-TiO2 catalyst. Based on the various characterization results, it is found that strong metal support interactions (SMSIs) are dominant on the Pd/r-TiO2 catalyst, which could facilitate the formation of oxygen vacancies and Pd2+ species in the active sites, resulting in excellent catalytic performance. This study not only improves the understanding of the distinctive structural properties of TiO2 crystal support but also offers an effective strategy to design efficient heterogeneous catalysts via tuning SMSIs.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2024
·Vol. 130
·期 10
·1-12
·
IF 2.5
Tang Mingxin,Qin Cong,Sun Xueya,Li Mengwei,Wang Yihui,Cao Jianliang,Wang Yan
Hydrogen (H 2 ) energy, as a clean energy source, has high energy density and durability, while H 2 is flammable and explosive, which requires strict safety technology measures to ensure the safety of high-pressure storage transportation. Therefore, the development of sensitive sensors is needed. In this study, In 2 O 3 microspheres with different Pd loadings were fabricated by hydrothermal method. Compared with the pristine In 2 O 3 gas sensor, the optimal operating temperature of the In 2 O 3 sensor is reduced from 160 ℃ to 80 ℃ after loading Pd. Among the prepared Pd/In 2 O 3 gas sensors, the response value of the 2 at% Pd/In 2 O 3 sensor towards 1000 ppm H 2 is 50.743 at 80 ℃. The response/recovery time is 80 s/235 s. The improved H 2 sensing performance can be ascribed to the chemical and electron sensitization of Pd, and the formation of PdO, PdH x . This study shows that Pd-loaded In 2 O 3 can effectively reduce the optimal operating temperature and enhance the response value for detecting H 2 in the range of 5-5000 ppm. Therefore, this sensor has good application prospects for detecting H 2 at low temperatures.
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TALANTA
·
2025
·
IF 6.1
Zhanhong Li,Mengyi Jiang,Dingxi Lu,Yuwei Wang,Haotian Li,Wen Sun,Jianjun Long,Itthipon Jeerapan,Jean Louis Marty,Zhigang Zhu
This study introduces a novel nonenzymatic glucose electrochemical sensor based on palladium-copper bimetallic aerogels (Pd–Cu BMA) synthesized through a facile self-assembly reduction method. The Pd–Cu BMA exhibits a three-dimensional network structure formed by interconnected nanowires, which facilitates rapid electron transfer and offers abundant active sites for catalysis. Benefiting from the synergistic effect of Pd and Cu, the Pd–Cu (2:1) aerogels demonstrates remarkable electrocatalytic activity and stability under neutral conditions. Specifically, this sensor achieves a rapid response to glucose oxidation at an applied potential of 0 V, with a linear detection range up to 20 mM and a limit of detection as low as 43.4 μM. Notably, it maintains high catalytic activity over one month and shows excellent anti-interference performance against common physiological interferents. For practical application, the sensor can accurately detect additional glucose in diluted serum within the concentration range of 1–20 mM and in undiluted serum from 1 to 4 mM, thereby validating its potential for real-time monitoring of glucose levels in physiological samples. This innovative design of Pd–Cu bimetallic aerogels not only enhances the performance of nonenzymatic glucose sensors but also paves the way for the development of advanced materials for point-of-care diagnostics.
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PubMed
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PETROLEUM SCIENCE AND TECHNOLOGY
·
2022
·
IF 1.695
Huili Zhang,Min Li,Jinjun Deng,Hailin Yu,Yanbin Tong,Lingmin Wu,Liqun Sun,Hongsheng Liu
Whether the oilfield sewage index can reach the reinjection specification is a crucial issue that is urgently need to be solved in polymer flooding systems. Thus the coagulability and floc morphology development of dual coagulants was systematically studied in different pH oily wastewaters. Acidification improved the deprotonation ability of coagulant. Hydrophobic associative polyaluminum silicate-poly dimethyl diallyl ammonium chloride (PASSC-PD) resolved the problem of excessive acid addition. The dual coagulants prepared not only preserved the high charge density of polyaluminum silicate (PASS) itself but also made it have the hydrophobic association and strong bridging ability. Besides, PASSC-PD was compared with hydrophobic associative polyaluminum silicate (PASS-C), PASS, and poly dimethyl diallyl ammonium chloride (PDMDAAC) pertaining to the polymer flooding oily sewage of Daqing Oilfield. The coagulation result demonstrated that PASSC-PD exhibited more advantageous turbidity and oil removal efficiencies than PASS-C, PASS, and PDMDAAC. The floc morphology result showed that adding dual coagulant made the petal-like floc of oily sewage larger at the pH value of 6. Furthermore relevant results evidenced that the coagulant had more successful fruits of turbidity removal of 96.5% and oil removal of 96.3% under weak acid conditions. These can satisfy the reinjection condition of oily sewage.
研究领域:
环境科学
·
化学工程
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DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Qing Zeng,Mengyuan Ma,Hui Liu,Lin Xu,Shaonan Tian,Dong Chen,Jing Wang,Jun Yang
Atomic surface engineering for nanostructures significantly contributes to the enhancement of electrocatalysis for a given chemical reaction. However, exploring a facile method to elaborately regulate surfaces at atomic scale remains a grand challenge. Herein, we report the construction of atomically rough surfaces (ARSs) on Au-based binary alloys through a novel and controllable gold (Au)-catalyzed strategy, which involves the first synthesis of Au-based bimetallic nanoalloys, i.e., AuPd and AuAg, and subsequent reduction of another metal ions (Pt, Pd, or Ag) initiated by Au sites on the alloy particle surfaces. By combining ARSs with low-coordinated atoms with ligand effect induced by vicinal Au atoms, the as-prepared ARSs exhibit good activity and durability toward ethanol oxidation reaction (EOR) in an alkaline medium. In particular, the Pd-Pt ARSs on the AuPd alloy particle surface (denoted as AuPd-Pt) exhibit the highest electrocatalytic EOR performance in terms of both specific activity (14.9 mA cm –2 ) and mass activity (28.5 A mg –1 ), surpassing those of their AuPd alloy counterparts, commercial Pd/C catalyst, and most Pd-based electrocatalysts reported recently. In situ Fourier transform infrared (FTIR) spectroscopy reveals that the EOR process on the Pd-Pt ARSs strongly prefers incomplete oxidation, which is further authenticated by the density functional theory (DFT) calculations.
研究领域:
材料科学
·
电化学
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PubMed
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JOURNAL OF ORGANIC CHEMISTRY
·
2021
·
IF 4.354
Quan Zhu,Yunsong Luo,Yongyan Guo,Yushun Zhang,Yunhai Tao
A highly efficient and practical Pd(II)/Cu(OAc)2-catalyst system of Saegusa oxidation, which converts enol ethers to the corresponding enals with a number of diverse substrates at extremely low catalyst loadings (500 mol ppm) under ligand-free and aqueous conditions, is described. Its synthetic utility was demonstrated by large-scale applications of the catalyst system to important nature molecules. This work allows Saegusa oxidation to become a highly practical approach to preparing enals and also suggests new insight into the Pd(II)/Cu(II)-catalyst system for dehydrogenation of carbonyl compounds and decreasing Pd-catalyst loadings.
研究领域:
有机化学
·
催化化学
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DOI
PubMed
高影响因子
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