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GREEN CHEMISTRY · 2023 ·Vol. 25 ·期 8 ·3198-3207 · IF 9.8

Achieving superior methanol oxidation electrocatalytic performance by surface reconstruction of PtNi nanoalloys during acid etching process

Xu Chen,Jinyu Zhao,Jie Lian,Xiaomin Wang

Developing and designing highly active and robust catalysts for the methanol oxidation reaction (MOR) are imperative towards the commercialization of direct methanol fuel cells. Herein, a Pt–Ni alloy catalyst (Pt1.5Ni-NGA) with ultrafine size (2.68 nm) and surface defects was designed and fabricated via a facile acid-leaching reconstruction strategy. The microstructural analysis showed that abundant surface defects were created in the Pt1.5Ni-NGA catalyst and are considered highly active methanol oxidation catalytic sites. Consequently, Pt1.5Ni-NGA exhibited a remarkable performance for MOR, achieving 6.3-times higher mass activity (MA, 1.88 A mg−1) in comparison with the commercial Pt/C catalyst (0.30 A mg−1). Simultaneously, Pt1.5Ni-NGA retained 79.8% of its initial MA after 10 000 s durability measurement in the acidic medium, demonstrating its improved durability. The experimental results revealed that the surface defects and modified electronic structure contributed to the enhanced MOR performance of Pt1.5Ni-NGA. This work offers a novel perspective for the rational construction of efficient Pt-based nanomaterials with defects for methanol oxidation.

研究领域: 材料科学 · 电化学 · 催化科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2018 · IF 3.141

Atomic Layer Deposition of a Pt-Skin Catalyst for Base-Free Aerobic Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid

Jinshan Shen,Hao Chen,Kequan Chen,Yong Qin,Xiuyang Lu,Pingkai Ouyang,Jie Fu

A Pt–Ni/AC bimetallic catalyst was prepared by atomic layer deposition of Pt nanoparticles on the surface of Ni/AC for base-free oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-furandicarboxylic acid (2,5-FDCA). A comparison of the Pt–Ni bimetallic catalyst with Ni and the Pt monometallic catalyst was demonstrated by X-ray diffraction (XRD), transmission electron microscopy (TEM), and temperature-programmed desorption of CO (CO-TPD). Compared with the Ni/AC and Pt/AC (1.6 wt % Pt) catalysts, the bimetallic Pt–Ni/AC catalyst had a higher activity for the oxidation of 5-HMF to 2,5-FDCA, with only a 0.4 wt % Pt loading. A 97.5% yield of 2,5-FDCA with 100% 5-HMF conversion was obtained after 15 h at 100 °C. A mass-based activity value of 35.8 h–1 was obtained over the Pt–Ni/AC-15ALD catalyst. The combination of Pt with Ni increased the ability of Pt for C═O adsorption and oxidation, thus increasing the activity of the Pt catalyst. Finally, the catalyst showed good reusability for at least four times without any reduction in the catalytic activity.

研究领域: 催化化学 · 材料科学 · 绿色化学
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Journal of Physical Chemistry C · 2017 · IF 4.536

Electrooxidation of Methanol on Pt @Ni Bimetallic Catalyst Supported on Porous Carbon Nanofibers

JianYi Chen,QiJian Niu,GuangKai Chen,Jun Nie,GuiPing Ma

This paper describes the preparation of Ni/Pt/CNFs via electrospinning technology, carbonization process, and chemical reduction method. The structure and composition of Ni/Pt/CNFs were characterized with X-ray diffraction, Raman spectroscopy, nitrogen adsorption isotherms, and X-ray photoelectron spectroscopy. Meanwhile, the morphology was analyzed with scanning electron microscopy and transmission electron microscopy. The electrochemical performance was evaluated by oxygen reduction reaction (ORR), cyclic voltammetry and chronopotentiometry. The results indicated that Pt and Ni nanoparticles were completely reduced in the experimental process and homogeneously distributed on the nanofibers with the average diameters of 3.8 and 17.8 nm, respectively. In addition, the Ni50/Pt/CNFs catalyst showed excellent electrocatalytic performance for ORR and superior specific and mass activities for methanol oxidation (the maximum current density is ca. 10.9 mA cm–2) and exhibited a slightly slower current decay over time, better than the reference samples which indicated a higher tolerance to CO-like intermediates.

研究领域: 材料科学 · 电化学
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Small Methods · 2025 ·Vol. 9 ·期 9 ·e00684 · IF 9.1

Tip-Enhanced Oxygen Reduction on Pt@Ni Cones via Concentrated Electric and Magnetic Fields

Guojun Han,Mohamed A. Tamerd,Ling Gao,Qingsheng Guo,Cong Feng,Menghao Yang,Guoxing Miao,Jing Fu

Efficient oxygen reduction reaction (ORR) is crucial for energy conversion technologies, yet its sluggish kinetics remain a significant challenge. Beyond optimizing the catalyst's intrinsic properties, field effects can also profoundly impact the microenvironment at the catalyst/electrolyte interface, thereby affecting electrocatalytic performance. This study explores the tip-enhanced ORR by leveraging the coupled effects of electric and magnetic fields at the reaction interface. The Pt-loaded ferromagnetic Ni cone electrode generates strong localized electric fields that reorganize interfacial water molecules into a more ordered structure. This strengthens hydrogen bonding between the electrolyte and reaction intermediates, which in turn facilitates proton-coupled electron transfer and accelerates the rate-limiting *OH desorption into interfacial water matrix. Additionally, the amplified electric fields at tips accelerate OH − electromigration away from the catalyst surface, while the migration current couples with the concentrated magnetic fields near tips to drive strong magnetohydrodynamic flows. These intensified flows effectively enhance O 2 molecule delivery to wider electrode surface and facilitate better OH − product removal, thus improving the overall reaction efficiency. This strategy of concentrating both E/M fields using the field-effect catalyst optimizes the ORR kinetics at the interface as well as the mass transport dynamics near interface, offering an effective approach for advancing ORR performance.

研究领域: 电催化 · 能量转换 · 纳米材料 · 物理化学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2020 · IF 4.65

The “electric-dipole” effect of Pt–Ni for enhanced catalytic dehydrogenation of ammonia borane

Bin Wang,Laifei Xiong,Hanjing Hao,Hairui Cai,Pengfei Gao,Fuzhu Liu,Xiaojing Yu,Chao Wu,Shengchun Yang

In this work, we prepared the PtNi alloy nanoparticles on Al 2 O 3 (Al 2 O 3 –PtNi) via a simple wet-grinding method followed by a thermal reduction process. The as-prepared Al 2 O 3 –PtNi displayed a higher TOF of 426.84 mol H2 (mol Pt ·min) −1 toward the dehydrogenation of AB (ammonia borane) than Al 2 O 3 –Pt and Al 2 O 3 –Ni. Based on the theoretical calculations, an “electric-dipole” effect generated by the neighboring Pt–Ni atoms was found to facilitate the catalytic dehydrogenation process of ammonia borane (AB). The external electric field produced by the Pt–Ni dipole can elongate the B–H bond and increase the negative charges of H atoms on the BH 3 group, which helps to activate the B–H bond in the AB molecule, and thus enhances the kinetic process of catalysis.

CAS / MDL: 7791-20-0
研究领域: 材料科学 · 化学工程 · 催化反应
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

High durability of Pt-Ni-Ir/C ternary catalyst of PEMFC by stepwise reduction synthesis

Rui Lin,Lu Che,Dandan Shen,Xin Cai

How to improve durability of catalysts is the major challenge hindering the large-scale implementation of proton exchange membrane fuel cells (PEMFCs). The alloy catalysts have been developed in efforts to reduce platinum loading, enhance catalysts activity and durability for oxygen reduction reaction (ORR) of PEMFCs. This manuscript reports the application of stepwise reduction synthesis to synthesize Pt–Ni/C and Pt–Ni–Ir/C catalysts. The synthesized electrocatalysts were characterized by X–ray diffraction (XRD), transmission electron microscopy (TEM), inductively coupled plasma mass spectrometry (ICP), X-ray photoelectron spectroscopy (XPS), cyclic voltammetry (CV) and linear sweep voltammetry (LSV). The results from CV and LSV showed that when as-prepared Pt–Ni–Ir nanocrystals are uniformly dispersed on the carbon support, the catalyst exhibits excellent electrocatalytic activity and stability. When the atomic ratio of Pt, Ni, Ir is 2:2:1, after durability test of 5000 cycles, rotating disk electrode (RDE) demonstrated ORR activities of the as-prepared catalysts with the highest mass activity (MA) of 351 m A ⋅ g P t − 1  at 0.9V iR-free and electrochemically active surface area (ECSA) of 80 m 2 ⋅ g P t − 1 , which is over 17 and 2 times than those of Pt/C JM (Johnson Matthey) catalyst, respectively. This work highlights the potential to use a preparative method which means step-by-step reduction synthesis to form ternary alloy catalysts for ORR of PEMFCs.

研究领域: 电化学 · 材料科学 · 纳米催化 · 能源材料 · 燃料电池技术 · 表面科学 · 电催化
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Amperometric H2S sensor based on a Pt-Ni alloy electrode and a proton conducting membrane

Weijia Li,Xinyu Yang,Yueying Zhang,Xidong Hao,Tong Liu,Xishuang Liang,Fangmeng Liu,Xu Yan,Fengmin Liu,Yuan Gao,Jian Ma,Geyu Lu

In this work, carbon fiber carrying platinum-nickel alloy is used as a sensing electrode material to develop a H 2 S gas sensor based on Nafion proton membrane. Characterizations of the material by X-ray diffraction (XRD), scanning electron microscope (SEM) and Energy Dispersive Spectrometer (EDS) reveal that the structure and morphology of the particles change with the ratio of the alloy. The electrochemical specific area (ECSA) of the material is calculated by cyclic voltammetry, which further proves the influence of alloy formation on the catalytic performance of the materials. When the ratio of platinum to nickel is 1:1, the material is uniformly loaded and its catalytic performance is optimal. Thus, the device made with it has the highest sensitivity. The sensor's low detection limit is 0.2 ppm. For the incorporation of nickel, the sensitivity is increased to -0.306 μA/ppm, which is 18 % higher than before. Not only does the sensor have good repeatability and short response recovery time, the presence of oxygen and water vapor does not have much effect on the sensor. Therefore, it has a great application potential in the field of gas detection at room temperature.

研究领域: 材料科学 · 电化学 · 气体传感技术 · 环境监测
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CATALYSIS LETTERS · 2024 · IF 2.3

Selective Hydrogenation of 5-Hydroxymethylfurfural to 2,5-bis(hydroxymethyl)furan by Pt/Ni@C Catalyst

Xu Xian,Lan Ling,Xu Jiangong,Liang Zheng,Tan Jin,Wang Haiyong,Qiu Songbai

The development of biodegradable materials from biomass is a crucial strategy for leveraging biomass resources. A key component in this process is 2,5-bis(hydroxymethyl)furan (BHMF), a significant biomass-derived platform chemical. However, producing BHMF with high selectivity through the selective hydrogenation of 5-hydroxymethylfurfural, while avoiding the creation of unwanted byproducts, is a complex challenge. In our research, we have developed a novel catalyst featuring a magnetic core. This catalyst, which consists of platinum loaded onto a graphene-like shell, has been applied to the catalytic hydrogenation of HMF in an aqueous environment. Under the optimized conditions of 373 K, 3 MPa H 2 , and 1 h reaction time, a BHMF yield exceeding 99% was achieved. This method presents a promising and effective approach for the high-value conversion of biomass waste into polymer materials and pharmaceutical chemicals. Graphical Abstract

CAS / MDL: 67-47-0 12054-48-7
研究领域: 化学工程 · 催化科学 · 可再生资源转化
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Russian Journal of Physical Chemistry A · 2022 ·Vol. 96 ·期 9 ·1935-1943 · IF 0.791

Highly Efficient Hydrogen Production from Ammonia Borane over Carbon Nanotubes Supported Pt–Ni Bimetallic Catalyst

Zhang Hui,He Jin,Lei Bowen,Wen Jie,Jing Fangli,Ali Arshid Mahmood

Abstract The bimetallic Pt–Ni nano-catalysts with different platinum to nickel mass ratios supported on the carbon nanotubes (PtNi( x  :  y )/FCNTs-D) were successfully synthesized by the polyol method and applied to the H 2 generation from ammonia borane (AB) hydrolysis. Several state-of-the-art characterization methods were performed to explore the correlation between catalytic performance and the physicochemical characterizations of the catalysts. The results show that the optimum Pt : Ni ratio is critical to enhance the H 2 generation from AB hydrolysis and in this study, it is 1 : 2. The presence of carbon nanotubes enhanced the dispersion and stability of the Pt–Ni nanoparticles. The availability of more active sites and lowered binding energy of Pt 0 in PtNi(1 : 2)/FCNTs-D catalyst, lead to the increased catalytic activity of H 2 generation from AB hydrolysis.

研究领域: 化学工程 · 材料科学 · 催化反应
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ACS Catalysis · 2019 · IF 12.221

Impact of Heat Treatment on the Electrochemical Properties of Carbon-Supported Octahedral Pt–Ni Nanoparticles

Fei Xiao,Xueping Qin,Mingjie Xu,Shangqian Zhu,LiLi Zhang,Youngmin Hong,Sang-Il Choi,Qiaowan Chang,Yuan Xu,Xiaoqing Pan,Minhua Shao

Thermal annealing is commonly used to remove surface contaminants and redistribute elements in alloys. In this study, Pt–Ni alloy nanoparticles supported on carbon black are selected as a model catalyst to understand the relationship between the annealing conditions (temperature and atmosphere) and the electrocatalytic performance for oxygen reduction, hydrogen evolution, and ethanol oxidation reactions. The impacts of thermal treatment temperature and atmosphere on structures, compositions, and in turn electrocatalytic activities are systematically studied. Interestingly, an ultrathin carbon layer can be formed on the nanoparticle surface by heat treatment in Ar atmosphere at temperatures higher than 350 °C, which significantly decreases its activity toward oxygen reduction and ethanol oxidation reactions. This carbon coating, however, is absent in other atmospheres including N2, air, 7% H2/Ar, and vacuum. Aberration-corrected scanning transmission electron microscopic characterizations with atomic-level resolutions confirm the formation of a Ni-enriched surface on Pt–Ni/C after treatment in Ar, which plays a critical role in catalyzing the growth of stable carbon layers from the surrounding carbons. Further density functional theory calculation results suggest that the absence of a carbon layer in N2 may originate from the stable N–C bond formed during heat treatment and passivation effect of adsorbed N2. It illustrates different effects of inert gases on carbon layer formation by combining experimental and computational approaches. These results may shed light on the proper design of postheat treatment protocols for carbon-supported catalysts and may also provide a feasible method to coat carbon layers on nanoparticle surfaces for various energy storage and conversion applications.

CAS / MDL: 7601-90-3
研究领域: 材料科学 · 电化学 · 催化
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 6 ·064513 · IF 4.316

Pt/Ni Catalyst Supported by Composite of Graphene and Polyaniline Microtubes Boosting Methanol Electrochemical Oxidation

Yunyi Xu,Wen Jin,Tingting Yu,Feng Wang,Xiaoyu Guo,Yiping Wu,Ye Ying,Ying Wen,Haifeng Yang

The development of durable and efficient anode electrocatalysts is crucial for direct methanol fuel cells. In this paper, polyaniline (PANI) microtubes are firstly prepared by removing the polystylene (PS) core from PANI coated electrospun PS. The catalyst of PtNi/PANI@rGO is built by two steps: graphene oxide (GO) is mixed with PANI microtubes to obtain PANI@GO and then PANI@GO is used as a support material to load PtNi nanoparticles by reductive reaction while GO is reduced into rGO. The morphology, electronic structure and chemical structure of the catalysts are characterized by SEM, TEM, XPS and Raman spectroscopy, respectively. The electrochemical analysis of electrochemical impedance spectroscopy, cyclic voltammetry and chronoamperometric measurement are performed to analyze the electrocatalytic performance. The electrochemical results indicate that as-synthesized PtNi/PANI@rGO has the high activity toward methanol oxidation, and its mass activity is 1.7, 1.3 and 4.1 times higher than that of PtNi/PANI, PtNi/rGO and commercial Pt/C catalysts, respectively. The PANI microtubes not only improve the electron transfer kinetic but also help avoid the accumulation of graphene layers. The doping of Ni into Pt changes the surface electronic structure to elevate the catalytic activity and helps effectively improve the resistance to CO poisoning.

CAS / MDL: 9003-53-6
研究领域: 材料科学 · 电化学
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2021 ·Vol. 26 ·期 2 ·481-490 · IF 2.647

Pt-Ni alloy catalyst supported on carbon aerogel via one-step method for oxygen reduction reaction

Jiang Li-Li,Zeng Min,Wang Chao-Yang,Luo Zhi-Hui,Li Hai-Yang,Yi Yong

Carbon-supported platinum-nickel alloy catalysts have become one of the main choices of proton exchange membrane fuel cells (PEMFCs) due to the high catalytic activity toward oxygen reduction reaction (ORR). In this work, carbon aerogel supported platinum-nickel solid solution alloy catalysts (Pt 3 Ni/CA) with small particles (~ 3.5 nm) and uniform distribution were prepared via a simple one-step rapid reduction method during which no structure guide or stabilizer is added. In rotating disk electrode (RDE), the mass activity (MA, 0.25 A mg Pt −1 ) and specific activity (SA, 4.69 A m −2 ) of the optimized Pt 3 Ni/CA catalysts for ORR are nearly 3.8 times and 6.5 times that of the state-of-the-art commercial carbon-supported platinum catalysts (Pt/C, 0.07 A mg Pt −1 and 0.72 A m −2 ), respectively. After the accelerated durability test (ADT), the as-prepared Pt 3 Ni/CA catalysts still keep a satisfactory MA and SA which are more than 3.4 and 8.9 times as high as that of Pt/C. The Koutecký-Levich (K-L) equation shows that the electrochemical reaction conforms to be a 4e − process.

研究领域: 材料科学 · 电化学
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