JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Chao Zhang,Yongsheng Gao,Haipeng Wang,Lulu Jiang,Delu Zhang,Shujun Ming,Guangying Fu,Chao Wang,Zhiguo Lv
The dry reforming of methane (DRM) could convert CH 4 and CO 2 into syngas, offering potential for greenhouse gas mitigation. However, DRM catalyst sintering and carbon deposition remain major obstacles. In this study, a highly dispersed PtNi alloy@Zr-doped 3D hollow flower-like MgAl 2 O 4 (AMO) spheres was prepared through a hydrophobic driving strategy. During a 50-hour test at 550 °C, the catalyst exhibited no significant decline in CH 4 and CO 2 conversion rates, demonstrating its excellent anti-sintering and anti-coking performance. The unique anti-coking performance can be attributed to Zr-induced oxygen vacancies, which enhance oxygen mobility and reduce carbon deposition. Besides, doped Zr increases basic active sites, enhancing CO 2 adsorption and activation, thus accelerating carbon species conversion. At 700 °C, the unique synergy between highly dispersed Pt and Ni enabled CH 4 and CO 2 conversion rates to reach 67.5 % and 73.8 %, respectively. The incorporation of Pt or Zr extends the Ni–Ni bond and partially coordinates with Ni, enhancing the stability of the Ni lattice. The reaction of CH 4 and CO 2 follows the Langmuir-Hinshelwood (L-H) mechanism, where both reactant molecules are adsorbed and activated on the metallic sites. Moreover, the effective energy barrier for the CH oxidation pathway is lower by 0.16 eV than that for the C oxidation pathway, which helps suppress the formation of carbon deposits.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Huixia Li,Shaofan Fang,Junfang Ding,Shaoqing Chen,Liping Li,Guangshe Li
Active-sites play a pivotal role in catalyzing reactions at surfaces, yet engineering these active sites still remains a significant challenge. In this work, hydroxylated MgO nanosheets supported ultrasmall PtNi alloys approximately 2.6(1) nm ( x Pt- y Ni/MgO hydr ) has been investigated via active-site engineering. Experimental results and DFT calculations reveal that electron transfers from Ni to Pt and from hydroxyl groups to Pt 5d-orbitals generate active sites NiPt-(OH) x . In the preferential CO oxidation (CO-PROX) reaction, these active sites on x Pt- y Ni/MgO hydr switch the bicarbonates reaction pathway depending on temperature range. Consequently, the optimal catalyst, 5%Pt-0.5%Ni/MgO hydr , achieves 100% CO conversion at 100 °C, demonstrating a broad temperature operation window (100–200 °C) and excellent durability. The active site engineering approach presented in this study can promote the discovery of more excellent catalysts with the optimal reaction route for various applications.
研究领域:
催化化学
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材料科学
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 5
·e202202811
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IF 5.02
Xue-Qi Zhang,Yu-Xuan Xiao,Ge Tian,Xiong Yang,Yuan Dong,Fan Zhang,Xiao-Yu Yang
Graphical Corrosion control : A PtNi alloy with a composite morphology comprised of nanobranches and nanoparticles is described. The unique morphology of the PtNi alloy facilitates electron accumulation on Pt, which enhances its resistance to chloride corrosion and performance in electrocatalytic hydrogen production in seawater. A solvothermal method to prepare PtNi alloys that have differing morphologies is described. By adjusting the feed ratio of Pt and Ni precursors in this process, PtNi alloys with different compositions (Pt : Ni atomic ratio from 1 : 3 to 3 : 1) and morphologies (evolution from nanobranches to nanoparticles) are generated. The prepared Pt 48 Ni 52 alloy, which has a composite morphology comprised of nanobranches and nanoparticles, exhibits superior activity and durability towards the hydrogen evolution reaction (HER) in seawater compared to those of commercial Pt/C catalyst and other PtNi alloys that have different compositions and morphologies. The excellent seawater HER performance of Pt 48 Ni 52 is ascribed to its nanobranch/nanoparticle morphology that optimally facilitates electron accumulation on Pt, which enhances resistance to chloride corrosion in seawater.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Fuxu Han,Jia Wu,Peichuan Sun,Yuzhen Zhang,Feng Tan,Wei Li,Mingli Xu,Chungang Min,Jianhua Wang,Xikun Yang
Due to the difficulty in controlling thermodynamics and kinetics of the growth for branched bimetallic metal alloy nanocrystals in a solution system, understanding the growth mechanisms of this class of nanostructures is critical for their shape-controlled synthesis. Herein, we report an approach to control over shape of branched PtNi alloy nanocrystals by tuning the molar ratio of Pt to Ni in an oleyamine solution. The detailed analyses confirmed that the morphologies of PtNi alloy nanocrystals evolve from dendrites (less than 5 at% Ni) to multipods (5–10 at% Ni) to star shapes (10–20 at% Ni) and finally to polyhedrons (100 at% Ni) as the nickel content in PtNi alloy nanocrystals increase. During the morphology evolution, the growth mechanism changes from oriented attachment growth to a new mechanism combining oriented attachment and anisotropic overgrowth, then to kinetically controlled overgrowth and finally to thermodynamic control growth. More importantly, we find that the growth of branched PtNi alloy nanocrystals is always along the [220] direction, and the growth direction determines the number of branches in nanocrystals. Electrochemical results show that highly branched PtNi alloy nanocrystals exhibit significantly enhanced electrocatalytic activity and durability compared with commercial Pt catalysts. These in-depth findings will provide new hints to precisely control synthesis of highly branched PtNi nanocrystals.
研究领域:
材料科学
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化学工程
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 10
·5359-5369
·
IF 11.9
Lanqing Li,Wei Gao,Jianqi Ye,Haoxin Fan,Dan Wen
Metallic aerogels with the hierarchical porous structure are promising materials for various electrocatalytic reactions; however, the regulation of their morphology and components remains a great challenge. Herein, three-dimensional porous PtNi aerogels composed of PtNi alloyed nanotubes with the tunable diameter and wall thickness were designed through a nanoengineering strategy of gelation and post treatment. The factors affecting the morphology and the mechanism for the growth of the multi-metallic aerogels were systematically investigated during their synthesis. Benefitting from the original interconnected networks and PtNi alloyed hollow blocks, the PtNi nanotubular aerogels displayed remarkable mass activity compared to the commercial Pt/C towards the oxygen reduction and methanol oxidation reactions for methanol fuel cells. Furthermore, different multi-component nanotubular aerogels of RuNi, Au–PtNi, and Ru–PtNi were also successfully fabricated using this nanoengineering strategy as active electrocatalysts. Therefore, the controllable nanoengineering strategy is considered a general pathway to obtain multi-metallic nanotubular aerogels, further providing a new idea for the design of hollow metallic aerogels as efficient electrocatalysts for fuel cell applications.
研究领域:
材料科学
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电化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2024
·
IF 16.8
Jiarun Cheng,Chaojie Lyu,Hang Lei,Xueyan Li,Hongyue Zhu,Dan Zhou,Wenjie Mai,Yiming Liu
The regulatory mechanism of strong metal-support interaction (SMSI) is of great significance in improving the electrocatalytic performance for supported electrocatalysts. Here, PtNi alloy nanoparticles were deposited on N, F-codoped graphene-like carbon nanosheets (PtNi@NFGC) to construct a highly active interface for efficient methanol oxidation reaction (MOR), which solves the problems of high cost, poor activity and easy aggregation of Pt-based catalysts. Due to the high electrophilicity, F atoms doping into the carbon lattice can not only manipulate the electron structure and the state of the carbon skeleton, but also further trigger the stronger charge transfer between metal atoms and carbon support. Compared with single-doped PtNi@NGC, N, F-codoped PtNi@NFGC possesses a lower onset potential and methanol oxidation potential, higher methanol oxidation current and stronger CO tolerance. The results of the partial density of state (PDOS) simulation display that N, F-codoping promotes the electron transfer from Pt atoms to NFGC support, and leads to the d-band center shift upward, thus strengthening the oxidation degree of Pt active sites and increasing the composition of high-valent Pt x+ . In-situ Raman analysis and density functional theory (DFT) results expound that F atoms embedding observably enhances the adsorption energy of Pt active centers to *OH intermediates, which not only significantly improves MOR catalytic activity, but also achieves efficient methanol dehydrogenation and alleviates CO poisoning. This customization of metal-support interface interaction by heteroatom doping strategy opens up opportunities for designing efficient supported catalysts.
研究领域:
电化学
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xingzhao Wang,Jian Che,Tingyong Wang,Fengqi Xu,Dongxia Duan
Low intrinsic electrocatalytic activity and inferior conductivity limit the application of Ni/NC in acidic electrocatalytic hydrogen evolution reaction (HER). Herein, we prepared nitrogen-doped carbon nanosheet confined PtNi alloy electrocatalysts (PtNi/NC-10) using PtCl 6 2− electrostatic adsorption coupling melamine pyrolysis nitriding strategy. PtNi alloying was confirmed by the crystallinity decrease and lattice expansion of Ni/NC. The alloying and confinement effect of Metal-Organic Frameworks (MOFs) suppresses the oxidation and agglomeration of metal nanoparticles during pyrolysis, thus significantly reducing particle size, increasing specific surface area, and promoting the exposure of active sites. The strong electronic interaction between Pt and Ni optimizeds the surface charge distribution, enhancing the adsorption of H species on electron-rich Pt sites, thereby improving reaction kinetics. In addition, PtNi alloying improves the conductivity of the material, accelerating charge transfer and proton transport. Consequently, the prepared PtNi/NC-10 exhibits superior HER performance than Ni/NC in 0.5 M H 2 SO 4 solution, even comparable to commercial 20 wt % Pt/C, with the overpotentials of 35 mV at 0.01 A cm −2 . Furthermore, the electrocatalysts assembled PtNi/NC-10-CP‖RuO 2 -TFF proton exchange membrane (PEM) electrolyzer only requires 2.32 V cell voltage to achieve 1 A cm −2 , presenting practical application prospects. Our work provides a novel idea for designing efficient and stable MOFs confined to alloy-based HER electrocatalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Huijuan Guan,Yafei Zhao,Jun Zhang,Yang Liu,Siguo Yuan,Bing Zhang
Highly dispersed Pt-based nanoparticles with superior electrocatalytic selectivity and stability are urgently needed for non-enzymatic electrochemical detection of H 2 O 2 . Herein, we prepared PtNi alloy nanoparticles dispersed in N-doped carbon nanofibers (PtNi/NCNFs) by pyrolyzing electrospun nanofibers composites from polyvinyl pyrrolidone and Pt/Ni-based salts. Characterization results indicated that PtNi alloy nanoparticles (average 9.0 nm) were homogeneously dispersed and embedded in NCNFs porous matrix. The electrochemical tests suggested that PtNi/NCNFs(3:1) displayed the highest electrocatalytic activity for H 2 O 2 reduction compared with Pt/NCNFs, Ni/NCNFs and other PtNi/NCNFs samples. PtNi/NCNFs(3:1)-based sensor showed excellent analytical properties towards H 2 O 2 with wide linear range (0.5 μM–8 mM), high sensitivity (248.5 μA mM −1 cm −2 ), low detection limit (0.0375 μM), high selectivity and anti-interference, attributing to the highly dispersion of nanoparticles and synergistic effect between PtNi alloy nanoparticles and NCNFs. The PtNi/NCNFs-based sensor had superior reproducibility due to the uniformity of PtNi/NCNFs and good stability because of the embedded structure, which prevented the aggregation and detachment of nanoparticles during repeated uses. More interestingly, the as-fabricated sensor displayed satisfactory recoveries and relative standard deviation (RSD) for detection of H 2 O 2 in milk samples. The above results manifested that PtNi/NCNFs had potential to be selected as a candidate for fabricating non-enzymatic H 2 O 2 sensors.
研究领域:
材料科学
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分析化学
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yanshan Mo,Shouquan Feng,Tianqi Yu,Jinli Chen,Guangfu Qian,Lin Luo,Shibin Yin
PtNi alloy nanoparticles display promising catalytic activity for oxygen reduction reaction (ORR), while the Ostwald ripening of particles and the dissolution/migration of surface atoms greatly affect its stability thus restricting the application. Herein, the WO x -surface modified PtNi alloy nanowires (WO x -PtNi NWs) exhibiting enhanced ORR catalytic property is reported, which has high aspect ratio with the diameter of only 2 ∼ 3 nm. It is found that the WO x -PtNi NWs shows a volcano relationship between the ORR activity and the content of WO x . The WO x-(0.25) -PtNi NWs has the best performance among all the synthesized catalysts. Its mass activity (0.85 A mg −1 Pt ) is reduced by only 23.89% after 30k cycles durability test, which is much more stable than that of PtNi NWs (0.33 A mg −1 Pt , 45.94%) and Pt/C (0.14 A mg −1 Pt , 57.79%). Hence this work achieves an effective regulation of the ORR activity for PtNi alloy NWs by the synergistic effect of WO x on Pt.
研究领域:
催化
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材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 24
·5531-5538
·
IF 6.813
Hongliang Zhu,Roong Jien Wong,Xiangbowen Du,Leilei Du,Zhikang Jin,KaiCheng Qian,Junjie Song,Renhong Li,Wen Liu
Low-cost and highly active catalysts are attractive for catalysing formic acid (FA) dehydrogenation at room temperature. The PtNi alloy nanoparticles with the characteristic of lattice contraction and synergy effects were loaded on two-dimensional TiB2 by incipient-wetness impregnation. Compared to Pt/TiB2, the substitution of Ni reduces the amount of noble metal required, with the added advantage of significantly improving the catalyst activity by sixteen times. By investigating the various PtNi ratios, the Pt3Ni8/TiB2 (total metal loading = 2.0 wt%) catalyst was found to provide a low activation energy of 27.7 kJ mol−1 in 10.0 M FA aqueous solution at room temperature. This is the first example of using the alloy supported on TiB2 to achieve strong metal–support interaction (SMSI) to catalyse formic acid dehydrogenation at ambient temperature. XPS and TEM characterisation studies show that higher temperatures induced TiB2 to encapsulate the PtNi NPs, with the TiB2 surfaces serving as the active site for catalysing FA dehydrogenation. The catalytic activity of the obtained Pt3Ni8/TiB2 catalyst for the dehydrogenation of FA was much higher than those of its monometallic counterparts (Pt/TiB2 and Ni/TiB2) prepared by the same method, while demonstrating higher stability against agglomeration and CO poisoning. The excellent catalytic activity and stability of Pt3Ni8/TiB2 were mainly attributed to the presence of the SMSI effect of the catalyst. Additionally, the lattice distortion and local interactions within the ferromagnetic clusters of Pt3Ni8 alloy NPs created a synergistic effect, which resulted in an enhanced SMSI effect throughout the catalyst. This study introduces a new concept that magnetic Ni metal partially replacing noble metals can improve thermal stability and catalytic performance, while enabling facile catalyst recovery. Moreover, this research demonstrates that the controlled synthesis and rational design of 2D reticular crystal structure TiB2-supported alloy NPs may provide new opportunities to enhance the catalytic activity and improve the SMSI effect of noble metal-based nanostructures.
研究领域:
催化
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材料科学
·
化学工程
·
纳米技术
✓ 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）