Nanoscale
·
2019
·Vol. 11
·期 24
·11513-11520
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IF 6.97
Huan-Feng Wang,Jun-Feng Li,Xue-Xi Sun,Ji-Jing Xu
The design of a nanoporous cathode for Li–O2 batteries that can achieve high chemical stability and superior electrochemical performance remains a formidable challenge. A novel approach for the fabrication of nanoengineered PdNi alloys directly coated onto Ni nonwoven fabric (PdNi/NiNF) obtained through electrospinning has been proposed. On the basis of the contributions of the porous structure, the prepared metal-based cathodes can exhibit high chemical and mechanical stabilities, high catalytic activity, and high conductivity. In this design, the major side reactions were excluded when compared with popularly used carbon cathodes, and excellent cycling stability (266 cycles) could be achieved. The proposed cathode exhibited a high discharge capacity of 15 700 mA h g−1 at 500 mA g−1, which was 5 times higher than those reported for carbon-free cathodes.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Zhao Jiang,Xiang Gong,Shuyi Guo,Yanxin Bai,Tao Fang
The NECZ/12H-NECZ (N-ethylcarbazole/dodecahydro-N-ethylcarbazole) system is regarded as the most potential liquid organic hydrogen carrier. However, the low activity, selectivity of NECZ and high cost of catalysts for the dehydrogenation reaction restrict its efficiency and commercial applications. In this work, a series of bimetallic Pd-M(M = Cu, Ni)/SiO 2 catalysts were prepared and employed to enhance catalytic activity and selectivity of NECZ for the 12H-NECZ dehydrogenation reaction. Pd 3 Ni 1 /SiO 2 exhibited high catalytic performance with 100% conversion, 91.1% selectivity of NECZ and 5.63 wt% hydrogen release amount at 453 K, 101.325 kPa for 8 h. The TOF (turnover frequency) of Pd 3 Ni 1 /SiO 2 is enhanced by 42.4% compared with Pd/SiO 2 . Combined with the characterization analysis, it was found that adjusting the alloying degree or the alloy phase in the PdCu and PdNi bimetallic catalysts could significantly enhance the dehydrogenation activity and selectivity, which were dependent on the component of bimetallic catalysts . This work may provide theoretical guidance for designing the efficient and low-cost bimetallic catalysts for the dehydrogenation of 12H-NECZ, which could boost the commercial applications of liquid organic hydrogen carriers.
研究领域:
催化化学
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材料科学
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能源化学
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产品关联
DOI
高影响因子
ACS ES&T Engineering
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2022
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IF 0
Xiangyu Ma,Hui Xu,Zhang Liu,Yanfei Liu,Chen Wang,Meiqing Shen,Chun Du,Bin Shan
Catalytic oxidation is a valuable residual methane removal method, and Pd-based catalysts are the most robust and widely applied system. Yet, they suffer from poor stability in practical applications due to sintering and water poisoning. In this work, we prepared a high-performance PdNi/Al2O3 catalyst with PdO-NiO and PdO-NiAl2O4 dual interfaces. PdNi/Al2O3 showed excellent hydrothermal stability after aging at 750 °C, 10% H2O for 72 h, with the T50 remaining below 315 °C. In addition, compared to bare Pd/Al2O3, PdNi/Al2O3 exhibited a better low-temperature activity with a T50 of 287 °C, rivaling state-of-the-art Pd-based catalysts. Combining structural characterizations and DFT calculations, it was shown that dual interfaces promoted the activation of methane C–H bonds and suppressed the adsorption of surface water/hydroxyl groups and agglomeration of PdO particles. This study has provided new perceptions for exploring the influence of interfacial interactions and offered a route to synthesize high-stability palladium catalysts.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Na Ye,Yanxin Bai,Zhao Jiang,Tao Fang
In the work, the catalytic performance and reaction mechanism of methanol oxidation reaction(MOR) are studied for the bimetallic Pd x Cu y and Pd x Ni y catalysts in alkaline solution. The results reveal that the Pd 1 Ni 1 /C and Pd 1 Cu 1 /C bimetallic catalysts exhibit high catalytic activity 4.1 and 3.9 times higher than that of the commercial Pd/C catalyst. Combined with the X-ray diffraction (XRD), High-resolution transmission electron microscopy(HRTEM) and X-ray photoelectron spectroscopy (XPS) analysis, the charge transfer between Pd and Cu(or Ni) alters the electron density of Pd and enhances the anti-CO poisoning ability, which is confirmed by DFT (Density Functional Theory) calculations. The CO binding energy is weakened on various bimetallic surfaces compared with that on Pd(111), consistent with experimental results. A linear relationship exists between the CO binding energy and the catalytic activity on the bimetallic catalysts, indicating that the CO binding energy may be the potential descriptor for MOR in alkaline media .
研究领域:
催化化学
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材料科学
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Xiaoxu Xu,Yuxin Sun,Kexin Lv,Yao Liu,Zhangpei Chen,Yifan Ouyang,Jianshe Hu,Qifan Chen
Palladium-based non-homogeneous catalysts have attracted considerable attention due to their high catalytic efficiency and adaptability. However, they still face the challenges of long reaction routes and poor cycling stability. An economical, efficient, stable and environmentally friendly catalyst PdNi@CN was prepared by loading nickel-palladium nanoparticles onto nitrogen-doped carbon functionalized carrier material. The catalyst was thoroughly characterized using XRD, XPS , SEM, TEM , VSM, and ICP . PdNi@CN could efficiently catalyze the Suzuki coupling reaction (Iodobenzene and phenylboronic acid , 97 % yield, TON (Turnover Number)=1.62 × 10 2 , TOF (Turnover Frequency)=2.43 × 10 2 h -1 ). Furthermore, PdNi@CN exhibited high activity in the reduction of 4-nitrophenol (4-NP, K app =8.01 × 10 –2 s -1 ). After five cycles of catalysis, the conversion of 4-NP still reached 95 %, demonstrating the excellent structural stability and high catalytic performance of PdNi@CN.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Xingjie Guo,Peng Hong,Lu Yao,Xudong Liu,Zhicheng Jiang,Bi Shi
Selective conversion of lignin derivatives into value-added chemicals benefits to develop sustainable chemical engineering and material manufacturing. In this work, a hydrotalcite-supported PdNi bimetallic catalyst was synthesized by introducing Ni to promote Pd dispersion and adjust the charge distribution of the active center, which was used for the catalytic hydrogenation of lignin-derived aldehydes in water under mild conditions. At 30 ℃ and 2 MPa H 2 , PdNi/HT achieved 99 % of vanillin (VAN) conversion with 100 % selectivity of vanillyl alcohol (VAL), and most of the typical lignin-derived aldehydes could be hydrogenated over this catalyst. This catalyst was steady and could be recycled at least five runs. The introduction of Ni and the nanosheet structure of HT improved the dispersion of the metal particles, significantly reducing the metal particle size. Besides, the Pd δ− –Ni δ+ pair and the basic sites of HT facilitated the H 2 activation and the adsorption of the aldehyde groups of lignin-derived aldehydes on the catalyst surface, enhancing the hydrogenation efficiency and selectivity.
研究领域:
化学工程
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Ning Zhang,Jing Wang,Wen Zhang,Yingxiu Zhao,Zemeng Dong,Zexing Wu,Guang-Rui Xu,Lei Wang
Despite considerable efforts to study direct alcohol fuel cells (DAFCs), the development of efficient bifunctional catalysts for monohydric alcohol and polyhydric alcohols remains a great challenge. This work reports the preparation of self-supported PdNi dendrites on Ni foam (self-supported PdNi DNTs/NF) with a large specific surface area by a simple self-sacrificing template and hydrothermal method. The presence of NF with enrichment of nucleation sites is crucial for the generation of self-supported PdNi DNTs. The as-obtained self-supported PdNi DNTs/NF exhibits an excellent property for ethanol and glycerol electrooxidation with the mass activity of 2375.7 mA mg cat −1 and 2451.6 mA mg cat −1 , the specific activity of 10.07 mA cm −2 and 10.84 mA cm −2 , respectively, in alkaline media, which should attribute to abundant high-index facets and low-coordinated atoms on the edge of branches. Furthermore, the PdNi DNTs/NF exhibits outstanding long-term durability in the current–time test for 7200 s with superior anti-CO poisoning performance, possessing a potential application in DAFCs.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Hongjing Wang,Wenxin Wang,Qiqi Mao,Hongjie Yu,Kai Deng,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
Strain engineering is a prospective approach to enhance catalytic performance of electrocatalysts. Herein, we report a CO-confined growth method for the synthesis of tensile-strained PdNi bimetallene as bifunctional catalyst for hydrogen evolution reaction (HER) and formate oxidation reaction (FOR). Ascribed to electronic effect and strain effect derived from the introduction of Ni and ultrathin curved geometry, PdNi bimetallene possesses sufficient active sites and modulates the adsorption/dissociation of electrocatalytic intermediates, resulting in outstanding activity and stability for HER and FOR. In HER-FOR system, a low cell voltage of 0.51 V is achieved at 20 mA cm −2 by PdNi bimetallene, which is 1.21 V lower than that for the conventional water electrolysis. This work offers a versatile route for the synthesis of crimped bimetallene materials for advanced energy-efficient hydrogen production and beyond.
研究领域:
材料科学
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电化学
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催化
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2022
·
IF 4.654
Pu Wang,Xingyu Zhang,Run Shi,Jiaqi Zhao,Zeyu Yuan,Tierui Zhang
Steam methane reforming is one of the primary industrial hydrogen sources but depends upon high temperatures to activate the inert C–H bonds in methane, motivating novel methods to achieve more sustainable methane activation and hydrogen production. Here, we prepared a PdNi bimetallic catalyst derived from layered double hydroxides for light-driven steam methane reforming, achieving a hydrogen production rate of 82.9 mmol g–1 h–1 at 300 °C under xenon lamp illumination. Outdoor condensed sunlight irradiation further delivered a hydrogen production rate of up to 260.9 mmol g–1 h–1. Both temperature-programmed desorption and density functional theory calculations indicated that Pd doping enhances the adsorption and activation of inert methane molecules, promoting hydrogen production via the reforming process. These results provide a reference for the direct utilization of solar energy to produce hydrogen from earth-abundant natural gas and water sources.
研究领域:
化学工程
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材料科学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Haipeng Xiao,Hongyan Pan,Weiyue Zhao,Chunliang Yang,Zheng Chen,Mingrui Liao,Qian Lin,Song Li
The direct synthesis of hydrogen peroxide (DSHP) through the reaction of hydrogen and oxygen under atmospheric pressure offers a highly atom-economic and environmentally friendly approach. However, this process is hindered by low productivity and selectivity of H 2 O 2 . Inspired by the adhesive properties of mussels, we successfully developed a bimetallic nanocluster catalyst, Pd x Ni y /SiO 2 @PDA, leveraging strong metal-support interactions (SMSI) for enhanced catalytic performance. Among these, the catalyst Pd 0.7 Ni 0.3 /SiO 2 @PDA demonstrated exceptional catalytic activity, achieving H 2 O 2 productivity and selectivity of 7210.60 mmol/g Pd ·h -1 and 95.30 %, respectively—representing improvements of 319.51 % and 33.50 % over the unmodified Pd/SiO 2 catalyst (1718.84 mmol/g Pd ·h -1 and 61.80 %). The anchoring mechanism of phenolic hydroxyl and amino groups on the polydopamine (PDA) coating was systematically investigated using control groups modified with tea polyphenols (TP) and 3-aminopropyltriethoxysilane (APTES), rich in phenolic hydroxyl and amino groups, respectively. Characterization revealed that amino groups on the PDA layer served as the primary anchoring sites, and the phenolic hydroxyl and quinone groups play a role in optimizing the electronic structure of Pd in an electron-deficient state. Synchrotron-based X-ray absorption fine structure (XAFS) analysis and density functional theory (DFT) calculations further revealed that the incorporation of Ni, a metal with a smaller atomic radius and lower electronegativity, reduced the Pd-Pd interatomic distance and shift the d -band center downwards from -1.72 eV to -1.94 eV. This modification inhibited the dissociative adsorption of O 2 * at Pd sites, thereby significantly enhancing H 2 O 2 productivity and selectivity.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Jia Cheng,Yang Xiang,Xun Huang,Zidong Wei
Electrocatalytic oxidation of surplus ethylene glycol (EG) to high-value glycolic acid (GA) represents a promising approach for sustainable resource utilization, though critical challenges persist in developing durable electrocatalysts and achieving effective recovery of the free acid product from its salt derivatives in alkaline electrolytes. In this work, a PdNi/NF catalyst was rationally synthesized via a one-step electrodeposition method. Systematic characterization revealed that the electron transfer from Ni to Pd modulates *OH adsorption to accelerate EG oxidation reaction (EGOR) while preventing Pd deactivation through oxidation. The optimized system demonstrated exceptional alkaline performance with a glycolic acid Faraday efficiency of 95% and a current density of 666 mA cm -2 . When implemented in an asymmetric EGOR||HER flow cell configuration where only the cathodic electrolyte contains alkaline, the system demonstrated exceptional operational stability by sustaining 70 mA cm -2 current density at a low cell voltage of 0.9 V in neutral media for over 100 h, with product glycolic acid requiring no further acidification. This investigation provides a practical framework for designing efficient electrocatalytic systems that simplifies product separation steps.
研究领域:
电化学
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催化
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材料科学
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化学工程
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 23
·10856-10867
·
IF 9.931
Xiangzhong Ren,Moujie Huang,Shan Luo,Yongliang Li,Libo Deng,Hongwei Mi,Lingna Sun,Peixin Zhang
A novel free-standing and binder-free air electrode with excellent electrochemical performance was designed for highly reversible Li–O2 batteries. The 3D hierarchically N, S co-doped macro–mesoporous carbon (NSMmC) was deposited on carbon paper (CP) via a template method, and then uniformly decorated with PdNi nanoparticles. The macropores of the porous carbon can provide enough space to accommodate discharge products, while the interconnected pores and channels efficiently facilitate oxygen and electrolyte diffusion. The introduction of PdNi nanoparticles greatly reduce the charge transfer resistance, resulting in the improvement of electron mobility of the whole cathode. Compared with Pd–NSMmC/CP and NSMmC/CP cathodes, the PdNi–NSMmC/CP cathode shows considerable enhancement of Li–O2 battery performance. The ultrafine and evenly distributed PdNi nanoparticles can not only provide enough catalytic sites, but can also tailor the discharge products into a cage-like morphology, which provides enough channels for electron and lithium ion transport. Moreover, the smaller size of the cage-like Li2O2 makes it decompose more easily, resulting in lower charge overpotential. This study provides a promising strategy to design 3D structured air cathodes for Li–O2 batteries with high electrocatalytic performance.
研究领域:
材料科学
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电化学
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能源存储
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）