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LANGMUIR · 2015 · IF 4.457

Preparation of Janus Pd/SiO2 Nanocomposite Particles in Inverse Miniemulsions

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 · 纳米技术 · 催化化学 · 胶体与界面化学
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Applied Catalysis O: Open · 2024 · IF 0

Insight into complexation of Pd-catalyst for methoxycarbonylation of ethene

Si Xiong,Aiping Wang,Baohe Wang,Jing Ma,Zhaobang Zhang,Jing Zhu

The complexation of palladium with bidentate phosphine ligand has significant effects on the activity of the catalyst for methoxycarbonylation of ethene. Herein, the influence of the ratio of components, kind and sequence of additives, complexation temperature and time on the catalytic performance were studied, then probable mechanism was proposed, and further kinetic studies were carried out under the optimized conditions. Compared to add Methanesulfonic acid (MSA) after complexation, the addition of an appropriate dose of MSA before complexation rather than after complexation could effectively improve the activity of the catalyst, while the addition of Methyl Propionate (MeP) would reduce the activity of the catalyst. It was worth noting that the weak absorption of [Pd-H] + in 1943 cm −1 was captured in the complex by in situ FT-IR.

研究领域: 催化化学 · 有机化学
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JOURNAL OF HAZARDOUS MATERIALS · 2015 · IF 4.529

Highly active Pd–In/mesoporous alumina catalyst for nitrate reduction

Zhenwei Gao,Yonggang Zhang,Deyi Li,Charles J. Werth,Yalei Zhang,Xuefei Zhou

The catalytic reduction of nitrate is a promising technology for groundwater purification because it transforms nitrate into nitrogen and water. Recent studies have mainly focused on new catalysts with higher activities for the reduction of nitrate. Consequently, metal nanoparticles supported on mesoporous metal oxides have become a major research direction. However, the complex surface chemistry and porous structures of mesoporous metal oxides lead to a non-uniform distribution of metal nanoparticles , thereby resulting in a low catalytic efficiency. In this paper, a method for synthesizing the sustainable nitrate reduction catalyst Pd–In/Al 2 O 3 with a dimensional structure is introduced. The TEM results indicated that Pd and In nanoparticles could efficiently disperse into the mesopores of the alumina. At room temperature in CO 2 -buffered water and under continuous H 2 as the electron donor, the synthesized material (4.9   wt% Pd) was the most active at a Pd–In ratio of 4, with a first-order rate constant ( k obs   =   0.241   L   min −1   g cata −1 ) that was 1.3× higher than that of conventional Pd–In/Al 2 O 3 (5   wt% Pd; 0.19   L   min −1   g cata −1 ). The Pd–In/mesoporous alumina is a promising catalyst for improving the catalytic reduction of nitrate.

研究领域: 环境科学 · 材料科学
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JOURNAL OF CATALYSIS · 2020 · IF 7.888

Cu-Pd pair facilitated simultaneous activation of ethanol and CO

Jian Zhang,Yazhe Zhang,Jieqiong Zhao,Zhe An,Yanru Zhu,Xin Shu,Hongyan Song,Xu Xiang,Xiaodan Ma,Jing He

Oxidative carbonylation has attracted broad interest from both academia and industry in recent years. Oxycarbonylation of ethanol to diethyl carbonate (DEC) has been of great challenge due to the difficulty in the simultaneous activation of ethanol and CO. This work reports a heterogeneous Cu-Pd pair catalysis for simultaneous activation of ethanol and CO, affording a selectivity of 85.4% to DEC and a space–time yield (STY) of up to 207 mg∙g −1 ∙h −1 . Well distributed Cu-Pd pair affords more Cu (I) sites, promoting CO activation and the followed insertion to adsorbed ethanol. Further increasing ratio of Cu (I) species via the pre-treatment of catalyst with CO and ethanol promotes simultaneously the activation of ethanol and CO, affording a STY of 325 mg∙g −1 ∙h −1 of DEC.

研究领域: 化学工程 · 催化科学
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ACS Applied Nano Materials · 2024 · IF 5.3

Urchin-like Au/Pd Nanobranches for the Oxygen Reduction Electrocatalysis

Qiuxiang Wang,Junlin Cai,Yu Sun,Weizhen Chen,Hongpu Huang,Shupeng Wang,Luhong Fu,Shuifen Xie

Three-dimensional (3D) porous heterogeneous metallic nanomaterials hold remarkable competitiveness in electrocatalytic fields due to their flexible porous structure and the electronic effect between heteroatoms, but challenges in synthesis still remain. Here, we design a facile stepwise reduction method to successfully synthesize urchin-like Au/Pd nanobranches (NBs). In a one-pot synthesis, small Au nanoparticles were initially generated. Later, numerous Pd nanotwigs were epitaxially grown and interlaced on the Au seeds to create unique channels, forming an Au-core/Pd-branches structure eventually. The as-prepared Au/Pd NBs exhibit greatly improved activity and stability for alkaline oxygen reduction reaction (ORR) electrocatalysis compared to the commercial Pt/C, with mass activity (1.4 A mg–1) and specific activity (2.4 mA cm–2) increased by 8.8 and 8.9 times, respectively. The excellent ORR performances of Au/Pd NBs are mainly attributed to the optimized electronic structure, improved utilization of surface active sites, and accelerated mass and charge transfer, which derives from the strong ligand effect, as well as the abundant porous channels of the Au/Pd NBs structure. The controllable design and synthesis of 3D porous Pd-based nanomaterials sheds light on a gigantic potential for ORR electrocatalysis.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Pd-TiO2 Schottky heterojunction catalyst boost the electrocatalytic hydrodechlorination reaction

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 · 材料科学 · 催化化学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Atomic hydrogen-mediated enhanced electrocatalytic hydrodehalogenation on Pd@MXene electrodes

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.

CAS / MDL: 15307-86-5
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Journal of the American Chemical Society · 2023 · IF 15

Continuous Phase Regulation of a Pd–Te Hexagonal Nanoplate Library

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.

CAS / MDL: 32294-60-3 3375-31-3
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JOURNAL OF ALLOYS AND COMPOUNDS · 2017 · IF 3.133

Peptide capped Pd nanoparticles for oxygen electroreduction: Strong surface effects

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.

CAS / MDL: 10025-98-6 16940-66-2
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CHINESE JOURNAL OF CATALYSIS · 2013 · IF 1.304

Preparation of microcapsule-supported Pd catalyst using a microfluidic platform

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.

CAS / MDL: 1321-74-0 100-42-5
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING · 2024 ·Vol. 130 ·期 10 ·1-12 · IF 2.5

Enhanced H2 gas sensing performances by Pd-loaded In2O3 microspheres

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.

CAS / MDL: 7758-95-4
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NEW JOURNAL OF CHEMISTRY · 2025 · IF 2.5

Effects of crystal structure of TiO2 on Pd-based catalysts

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.

CAS / MDL: 13463-67-7
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