CATALYSIS LETTERS
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2019
·Vol. 150
·期 5
·1277-1286
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IF 2.372
Zou Zhijuan,Jiang Yaya,Song Kunpeng
Abstract Metalporphyrin-based porous polymers supporting high dispersed Pd nanoparticle (NP) catalysts (HUST-1-Pd) were prepared with a novel solvent-knitting hyper-crosslinked polymer method using 5-, 10-, 15-, and 20-tetraphenylporphyrin (TPP) as building blocks. The N 2 sorption isotherms of the catalysts show that the HUST-1-Pd possesses many ultra-micropores and continuous mesopores. The NPs are assembled on tetraphenylporphyrin structures and show Pd-N 4 composition-dependent catalysis for methanolysis of ammonia borane (AB) and hydrogenation of aromatic nitro compounds to primary amines in methanol solutions at room temperature. The nano-palladium reduced by NaBH 4 has efficient catalytic activity for AB methanolysis. A variety of R-NO 2 derivatives were reduced selectively into R-NH 2 via palladium catalyzed tandem reactions with 5–30 min of reaction time with conversion yields reaching up to 90%. The derivatives also give excellent recycling performance (more than 10 times). Furthermore, the turnover frequency (TOF) can reach 87,209 h −1 . The HUST-1-Pd compounds represent a unique metal catalyst for hydrogenation reactions in a green environment without using pure hydrogen. Graphic Abstract A monodisperse Pd NPs embed in porphyrin-based microporous organic polymer was reported to catalyse the tandem dehydrogenation of ammonia borane and hydrogenation of R-NO 2 to R-NH 2 at room temperature. The catalyst is efficient and reusable in an environment-friendly process with short reaction times and high yields.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2019
·
IF 1.911
Weiquan Cai,Junlin Zhuo,Jimin Fang,Zhichao Yang
A series of nanorod-like porous Pd/γ-Al 2 O 3 catalysts with controllable textural properties and enhanced catalytic performance in 2-ethyl-9,10-anthraquinone (eAQ) hydrogenation for H 2 O 2 preparation were successfully prepared via a facile sol–gel method using aluminum isopropoxide as aluminum precursor and eAQ as structure directing agent, sequential calcination and impregnation process with Na 2 PdCl 4 solution. The physicochemical properties of the catalysts obtained with different addition amounts of eAQ were comparatively characterized by XRD, TG–DSC, BET, TEM, CO-TPR, H 2 -TPR and H 2 –O 2 titration. The results show that addition of eAQ can not only effectively control the textural properties (surface area, pore volume and average pore size) of the catalysts, but also lower their reduction temperature of active metal. Importantly, the catalyst obtained with an addition amount of 4 wt% eAQ shows the highest hydrogenation efficiency of 10.28 g·L −1 , which is 37.3% higher than 7.49 g·L −1 of the catalyst obtained without eAQ.
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ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Guoqing Sheng,Jiahui Chen,Yunming Li,Huangqing Ye,Zhixiong Hu,Xian-Zhu Fu,Rong Sun,Weixin Huang,Ching-Ping Wong
Flowerlike NiCo2S4 hollow sub-microspheres are synthesized through Cu2O templates to support Pd nanoparticles as high-efficiency catalysts for the hydrogen evolution reaction (HER). The diameter and shell size of NiCo2S4 hollow sub-microspheres are about 400 and 16 nm, respectively. In addition, the surface of the shells is constructed by petallike nanosheets. About 3 nm Pd particles uniformly incorporate with the flowerlike NiCo2S4 hollow sub-microsphere to form the NiCo2S4/Pd heterostructure. The NiCo2S4/Pd catalysts exhibit significantly lower overpotential of only 87 and 83 mV at 10 mA/cm2 for the HER in both acidic and alkaline conditions, respectively, relative to NiCo2S4 (247, 226 mV) and Pd (175, 385 mV) catalysts. Besides, the NiCo2S4/Pd catalysts also exhibit excellent stability of HER in these two conditions. The superior HER performance of NiCo2S4/Pd might be resulted from the unique architecture of metal nanoparticles anchored on the bimetallic sulfide flowerlike hollow sub-microspheres, which could provide high surface area, lots of active sites, strong synergetic effect, and stable structure.
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PubMed
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
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2018
·
IF 4.66
Siliao Zhou,Xianghan Chen,Ping Yu,Feng Gao,Lanqun Mao
A highly efficient electrocatalyst for the hydrogen evolution reaction was developed using nitrogen-doped carbon nanotubes (N-CNTs) as a substrate for the electroless deposition of Pd nanoparticles (PdNPs). The N-CNTs were prepared with ionic liquid as a precursor through a programmed temperature method. The resulting PdNP@N-CNTs nanocomposite was characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS) and electrochemical impedance spectroscopy (EIS). Electrochemical experiments show that the nanocomposite has high electrocatalytic activity toward hydrogen evolution with a current density of 32 mA cm −2 at an overpotential of 100 mV and a low Tafel slope (33 mV/dec) with excellent stability. The high catalytic activity and durability were considered to be due to N atoms incorporated into the carbon skeleton forming numerous active sites for the deposition of small and uniformly distributed Pd nanoparticles. This work provides a new way to prepare highly efficient electrocatalysts for hydrogen evolution.
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CARBON
·
2018
·
IF 7.082
Yanli Huang,Qiuli Wei,Yuanyuan Wang,Liyi Dai
In this work, three-dimensional (3D) amine-terminated ionic liquid (IL) covalently functionalized graphene/Pd composite aerogels are successfully fabricated via a facile and green reduction-inducing self-assembly method. The morphology and composition of the obtained 3D IL-rGO/Pd composite aerogels are studied by means of TEM , SEM , XRD , FTIR , XPS , BET, and Raman spectroscopy . In those composites, the cations of NH 2 -IL introduced to the surface of graphene sheets can avoid the restacking of graphene sheets and enlarge the specific surface area, which provide efficient transport pathways for improving the catalytic performance. The negatively charged Pd precursors (PdCl 4 2− ) are adsorbed on positively charged imidazolium ring moiety of NH 2 -IL to engender Pd NPs with small particle sizes uniformly distributed on the graphene sheets, which can maximize the active surface area of catalysts and enhance their catalytic activity . The catalytic studies show that the 3D IL-rGO/Pd composite aerogels can be used as efficient, easy separation, recyclable, and stable catalysts for the Suzuki cross-coupling reactions under mild conditions, and the catalytic efficiency shows no obvious loss even after ten repeated cycles.
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Reaction Kinetics Mechanisms and Catalysis
·
2018
·Vol. 126
·期 1
·463-476
·
IF 1.515
Zhang Jiuxuan,Liu Yefei,Jiang Hong,Chen Rizhi
A highly efficient catalyst with the structure of semiconductor–metal heterojunction for phenol hydrogenation in water was fabricated by loading the Pd nanoparticles on the N-doped porous carbon-TiO 2 (CN-TiO 2 ) materials, which was synthesized via the one-step carbonization of TiO 2 -contained ZIF-67. The microstructures of the as-prepared Pd@CN-TiO 2 catalysts were investigated in detail and the catalytic properties were tested by the phenol hydrogenation under mild conditions. With increasing TiO 2 amount, the charge transfer and specific surface area of Pd@CN-TiO 2 initially increase and then reduce, thereby the catalytic performance show a similar regular pattern. The as-fabricated Pd@CN-TiO 2 exhibits a superior catalytic performance than the Pd nanoparticles supported on TiO 2 or CN separately, owing to their synergistic effect. When the parameters affecting the catalytic efficiency are optimized, the conversion of phenol and selectivity for cyclohexanone can even achieve 98% in pairs with a higher reaction rate of 0.45 mmol h −1 . Furthermore, the Pd@CN-TiO 2 shows stable performance in the recycling experiments.
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CHEMISTRY OF MATERIALS
·
2014
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IF 8.535
Na Lu,Wei Chen,Guoyong Fang,Bi Chen,Keqin Yang,Yun Yang,Zhencai Wang,Shaoming Huang,Yadong Li
We report that 5-fold twinned nanowires and single twinned right bipyramids of Pd with high yields can be selectively synthesized in a hydrophilic system with the assistance of acetonitrile and ethanol, respectively. The controlled synthesis is based on an idea that small organic molecules (SOMs) that can attract halide ions via electrostatic interactions of different strengths could well adjust their activity to tune the etching degree of O2/halides for protecting the twinned Pd crystal nucleus. We consider that relatively stronger interaction between acetonitrile and halide ions for the formation of nanowires is due to the existence of three C–Hδ+ bonds induced by the electron-withdrawing CN group of CH3CN, which is confirmed by an as-called iodine starch test, 1H nuclear magnetic resonance spectra, and theoretical calculations. On the basis of this finding, we then have successfully expanded SOMs to other molecules, including acetone, 1,4-dioxane, and 1,3,5-trioxane, which have a function similar to that of acetonitrile for the production of Pd nanowires, and 2-propanol, which has a function similar to that of ethanol for the fabrication of right bipyramids. Although nanowires and bipyramids are both mainly bound by {001} planes, nanowires show better catalytic performance toward the reduction of 4-nitrophenol, indicating that more twin boundaries could offer more active catalytic sites. This work not only provides new information to decrease the degree of etching of O2/halides for controlling twin structure of noble metals but also supports the idea that creating a twin structure is good for enhancing catalytic activity.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Fenglei Liu,Baowei Hu
Recovery of precious metal ions in wastewater could not only improve resource utilization, but also could reduce environmental pollution. Herein, a composite of TpPa@Nb 2 C was constructed by an interfacial self-assembled method and explored the synergistic adsorption effects for precious metals. The structure and morphology of the composites were analyzed by advanced characterization techniques, followed by parametric analysis of Au(III)/Pd(II) adsorption from the simulated wastewater. The results showed that the grafting of COFs with abundant reducing active sites on the MXenes could significantly improve the selectivity and adsorption capacity. Meanwhile, the interaction was found as monolayer way and controlled by chemistry process, and the maximum equilibrium Au(III) and Pd(II) uptake reached up to 910.1 and 386.2 mg/g, respectively. The competitive adsorption study showed that the co-existence of impurities had little effect on the removal rate. The mechanism analysis demonstrated that the precious metal ions were reduced to elemental gold/palladium on the network of TpPa@Nb 2 C, and they got three electrons or two electrons from the hydroxyl groups through redox reaction, respectively. Thus, this study provided an excellent material for enrichment and recovery of precious metals in waste liquid and the treatment of e-waste.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Long Jiang,Yaojie Liu,Lulu Zhang,Liang Qin,Zongjiang Yu,Mo Xian,Weizhi Sun,Chao Xu
How to quantitatively describe metal–ligand interactions is the key to design high-affinity ligand. In this study, the electron transfer ratio (ETR), which correlated 34 chemical ligands with the electron donating ability, allowed for obtaining six high affinity multidentate S/N-containing ligands, and the interactions were further analyzed by frontier orbital and electrostatic potential calculation. Furthermore, six corresponding ligand-modified polystyrene framework materials were prepared by efficient derivatization of isothiocyanates and primary amines. The optimal material CMPS-BD had an adsorption capacity up to 4.07 mmol/g with good tolerance to different organic solvents. CMPS-BD exhibited excellent adsorption efficiency in combination with kinetics, thermodynamics, selectivity and regeneration performance. Moreover, the remarkable practicability was achieved as the removal rate reached 99.8 %, and the residual Pd 2+ concentrations were reduced to less than 5 mg/L in three kinds of Pd-catalytic reaction waste liquids. Through mechanism analysis, 1 mmol ligand FA ∼ BD could bind 0.75 ∼ 1.74 mmol Pd 2+ which was consistent with the ETR tendency, certifying the accuracy and efficiency of this method. Intensive DFT calculations revealed that the optimal ligand BD could generate a variety of spontaneous endothermic intermolecular and intramolecular coordination reactions.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2025
·
IF 7.8
Ruoyi Li,Muchen Lu,Jiaqi Yu,Jian Zhang,Jia Li,Xinyan Wang
Tigecycline (TGC), a third-generation, broad-spectrum, potent antimicrobial drug based on a tetracycline structure, may pose potential hazards to ecosystems and human health due to its difficulty in natural degradation in the environment. However, the environmental degradation behavior of TGC has not been fully investigated, so it is still a major challenge to rationally design efficient, stable, environmentally friendly and cost-effective electrocatalysts for TGC degradation. In this study, Pd-ZnS NPs/CF composite electrode anchored on copper foam (CF) was synthesized by simple ultrasonic method and two-step electrodeposition. The degradation efficiency of TGC at the Pd-ZnS NPs/CF composite electrode was as high as 88.75 % within 30 min under neutral conditions, and the energy consumption was only 0.11 kWh/m³ . In addition, the overall Pd 2+ contribution was as low as 0.00005 M after the introduction of inexpensive ZnS. The Pd-ZnS NPs/CF composite electrode exhibited excellent electrocatalytic activity and degradation of antibiotics under different aqueous environmental conditions. Suitable for degradation of a wide range of antibiotics with excellent cyclic stability. The TGC degradation rate was stabilized above 85.40 % after 240 min of continuous operation in a continuous flow reactor, and the composite electrode prepared once can be used for a long time. It highlights the broad application prospects of the composite electrode in the field of water treatment technology and the significant advantages of high efficiency, low energy consumption and stable long-term operation. In this study, the mechanism of action of ·OH and H* with TGC is also deeply investigated, and the dynamics of TGC degradation intermediates are probed using two-dimensional correlation spectroscopy (2DCOS) and density-functional theory (DFT) calculations. Finally, the ecotoxicity of Pd-ZnS NPs/CF composite electrodes is investigated, which provides a simple and feasible idea for the preparation of efficiently degraded antibiotic cathodes.
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Small
·
2025
·
IF 12.1
Wenli Lei,Shuang Zhang,Jiaxi Shu,Fudong Li,Zixuan Deng,Juejing Liu,Xiaofeng Guo,Yuanmeng Zhao,Changsheng Shan
Self-powered biosensors (SPBs) based on biofuel cells (BFCs) use electrical output as a sensing signal without the need of external power supplies, providing a feasible approach to constructing miniaturized implantable or portable devices. In this work, a novel nanozyme of gold nanoclusters/palladium nanocubes (AuNCs/PdNCs) heterostructure is successfully fabricated to develop an innovatively self-powered and non-enzymatic glucose sensing system. The AuNCs/PdNCs with glucose oxidase (GOD)-like activity exhibits superior electrocatalytic and non-enzymatic sensing performance toward glucose. The non-enzymatic BFCs-based SPBs system, established on the AuNCs/PdNCs (anodic catalyst) and single atomic Fe sites coupled with carbon-encapsulated Fe 3 C crystals (Fe 3 C@C-Fe SACs as a cathodic catalyst) platform, exhibits an exceptional sensitivity to glucose with 0.151 µW cm −2 m m −1 (3.4 times higher than the PdNCs), outstanding selectivity and robust stability. The outstanding performance of the BFCs-based SPBs system can be attributed to the synergistic cooperation between the PdNCs and AuNCs.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Qiao Ding,Ning Li,Bo Wu,Qing Cheng,Qi Zhao,Tong Liu,Rui Wang,Deyu Li
In this study, SO 2 was used to chemically modify the commonly used leveling agent polydimethyldiallylammonium (PD) in through-hole electroplating, resulting in a more effective leveling agent, PDS, which improved the throwing power (TP), leading to through-hole circuit boards with better metal coverage in difficult-to-reach areas. Furthermore, theoretical and experimental studies were conducted to understand how the −SO 2 structure influences the leveling ability of the leveling agent. The study demonstrates that the −SO 2 -modified additive significantly enhances the copper plating process, resulting in thicker and more uniform deposits in through-holes, which are critical for ensuring high-quality circuit boards.Additionally, this study elucidates the mechanism of action of the leveling agent on the copper surface, providing theoretical support for the development of copper plating leveling agents. The leveling ability differences between the leveling agents PD and PDS were investigated using Cyclic Voltammetry, constant current method, and Electrochemical Impedance Spectroscopy. Additionally, the optimal concentrations of the additives were determined. Quantum chemical calculations were employed to analyze the electrostatic potential, HOMO/LUMO orbitals, and differential charge density on the Cu (111) surface for both leveling agents. These theoretical analyses provided insights into the reasons behind the differing leveling abilities of the two agents.
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