JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2022
·
IF 4.383
Shaohui Zhang,Hao Cui,Haikun Zhou,Xiyu Tan,Pengfei Tan,Jun Pan
Platinum-based alloy nanowires are often employed in oxygen reduction reaction (ORR) due to their exceptional performances. However, most platinum-based alloy nanowires suffer from poor stability in strong acidic electrolytes, as well as their complex preparation methods. Herein, PtMn@Pt core-shell nanowires were successfully prepared by one-step hydrothermal with different concentrations of polyvinylpyrrolidone (PVP) and replacement reaction. The results show that the microstructure of nanowires gradually change with the increase of PVP concentration. Meanwhile, the outer layer of the PtMn nanowires contains a Pt-skin of about 1–2 nm. Moreover, the mass activity of the prepared PtMn@Pt core-shell nanowires with 50 mg PVP is 0.409 A mg −1 (@0.9 V), which is 3.86 times higher than that of commercial Pt/C. The as-prepared nanowires display excellent stability mainly due to the existence of Pt-skin. This paper provides a relatively simple method to synthesize Platinum-based core-shell nanowires with outstanding ORR performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xiao-Feng Han,Nadia Batool,Wen-Tao Wang,Hao-Tian Teng,Li Zhang,Ruizhi Yang,Jing-Hua Tian
Simple and reliable mass production of platinum-based alloy catalysts with excellent activity and stability is an enormous challenge for the wide commercialization of proton-exchange membrane fuel cells (PEMFC), especially those with ultralow loading of Pt. Herein, an economical, highly durable, and efficient catalyst consisting of structurally ordered intermetallic Pt3Co alloy nanoparticles with ultralow Pt loading (1.4 wt %) supported on hierarchically porous carbon structure (three-dimensional, 3D Pt3Co/C) were synthesized with large-scale production by the NaCl-template-assisted approach. The obtained best sample, 3D Pt3Co/C#1, exhibited mass activities of 11.56 and 0.70 A mgPt–1 for oxygen reduction reactions (ORRs) in alkaline and acidic electrolytes, which are 60.8 and 6.4 times those of commercial Pt/C, respectively. Furthermore, the 3D Pt3Co/C#1 exhibited excellent stability both in acidic and alkaline electrolytes, with almost no decay of the half-wave potential after 5000 potential cycles. This work proposes a new high-yielding, simple, and environmentally friendly method to fabricate excellent Pt-based alloy electrocatalysts with ultralow loading of Pt, which opens up new hopes for the development of PEMFC.
研究领域:
材料科学
·
电化学
·
燃料电池
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 31
·15882-15888
·
IF 7.443
Jing Sun,Haifeng Ma,Hong Jiang,Liyun Dang,Qingyi Lu,Feng Gao
We developed a one-step method to obtain a high dispersion of Pt-based alloy nanoparticles on graphene by using both the carrier function and the reducibility of carbon without the addition of any other reducing agent. This method opens up a general and feasible route for the synthesis of different metals, and binary and ternary alloys (such as Pt, Pt–Cu, Pt–Ni, Pt–Ni–Cu, Pt–Co–Cu, Pt–Au–Cu, and so on) on graphene sheets, which would bring potential applications in many fields. Particularly in this study, the obtained PtCu/G composites exhibit superior electrochemical activities and high poison tolerance toward methanol oxidation compared to Pt/graphene and commercial Pt/graphene composites, demonstrating that PtCu/graphene can be used as a promising catalyst for direct methanol fuel cells.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
Small
·
2024
·
IF 13
Yuxin Gao,Hang Liu,Xintian Wang,Xiao Liu,Bin Shan,Rong Chen
Pt-based alloy with high mass activity and durability is highly desired for proton exchange membrane fuel cells, yet a great challenge remains due to the high mass transport resistance near catalysts with lowering Pt loading. Herein, an extensible approach employing atomic layer deposition to accurately introduce a gas-phase metal precursor into platinum nanoparticles (NPs) pre-filled mesoporous channels is reported, achieved by controlling both the deposition site and quantity. Following the spatially confined alloying treatment, the prepared PtSn alloy catalyst within mesopores demonstrates a small size and homogeneous distribution (2.10 ± 0.53 nm). The membrane electrode assembly with mesoporous carbon-supported PtSn alloy catalyst achieves a high initial mass activity of 0.85 A mg Pt − 1 ${\mathrm{mg}}_{\mathrm{Pt}}^{-1}$ at 0.9 V, which is attributed to the smallest local oxygen transport resistance (3.68 S m −1 ) ever reported. The mass activity of the catalyst only decreases by 11% after 30000 cycles of accelerated durability test, representing superior full-cell durability among the reported Pt-based alloy catalysts. The enhanced activity and durability are attributed to the decreased adsorption energy of oxygen intermediates on Pt surface and the strong electronic interaction between Pt and Sn inhibiting Pt dissolution.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2022
·Vol. 9
·期 14
·2104927
·
IF 17.521
Yafeng Zhang,Kai Ye,Qianru Liu,Juan Qin,Qike Jiang,Bing Yang,Feng Yin
Structure-controlled Pt-based nanocrystals have the great potential to provide a flexible strategy for improving the catalysis of the oxygen reduction reaction (ORR). Here, a new synthetic approach is developed to tune the 3D structure of Pt-based alloys, and switch a synthetic reaction which produces solid PtCu octahedral stars (OSs) to produce PtCu nested skeleton cubes (NSCs) by simple addition of Ni(acac) 2 . In particular, Ni 2+ -guided anisotropic growth is observed to generate the nested skeleton structure in PtCu NSCs. Ni 2+ , though absent from the nanoalloys, not only endows faster Cu reduction kinetics but also acts as a structure-directing agent. Moreover, it is shown that acetic acid treatment of PtCu NSCs/C exposes Pt-rich surface with a fine-tuned Pt d-band center energy and the reduced Cu leaching, resulting in strikingly high activity and stability. Acid-treated PtCu NSCs/C shows a remarkable ORR mass activity of 5.13 A mg Pt –1 , about 26 times higher than commercial Pt/C catalyst. This catalyst also exhibits excellent stability with a lower activity decay of 11.5% and the negligible variation in structure after 10 000 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Yu Zhang,Qin Zhao,Bukhvalov Danil,Weiping Xiao,Xiaofei Yang
The Pt-based alloys can moderate the binding energies of oxygenated species on the catalytic surface, endowing the superior catalytic performance towards oxygen reduction reaction (ORR). Nevertheless, it is still challenging to explore general methods to synthesize structurally ordered intermetallics with uniform distributions. Herein, the strong metal-support interaction is employed to facilitate the interdiffusion of Pt/M atoms by establishing a tunnel of oxygen vacancy on ultrathin Ti 3 C 2 T x (MXene) sheets, synthesizing the ordered PtFe, PtCo, PtZn, PdFe, PdZn intermetallics loaded onto Ti 3 C 2 T x . Furthermore, the in-situ generation of Ti–O from Ti 3 C 2 T x could be bonded with Pt and forming Pt–O–Ti, resulting in charge redistribution through Pt–O–Ti structure. Theoretical calculations demonstrate that the valuable charge redistribution can be observed at the interface and extended even to at the distance of two nanometers from the interface, which can modulate the Pt–Pt distance, optimize Pt–O binding energy and enhance intrinsic activity towards ORR. The strong coupling interaction between PtFe and Ti 3 C 2 T x containing the titanium oxide layer endows the high stability of the composites. This work not only presents a general synthesis strategy for intermetallics but also provides a new insight that metal-support interaction is essential for the structural evolution of intermetallics on materials with oxygen vacancies.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Pengtao Qiu,Jinglei Bi,Xiaojing Zhang,Shengchun Yang
We present a novel synthetic strategy for the shape-controlled synthesis of Pt-based alloy nanoparticles (NPs) in inorganic molten salt without using any organic surfactants or capping agents. Graphene oxide (GO) was chosen as the stabilizer in the inorganic molten salt synthetic strategy, due to the existence of various oxygen-containing functional groups on its surface, which adsorb, anchor, and stabilize the metal ions or NPs. After GO was added in molten salt, the PtPd nanosheets were formed on its surface in H2 atmosphere. In addition, when KI was chosen as the shape-inducing agent to selectively adsorb on and fully protect the (100) facets of alloys, PtPd nanocubes with core–shell structure, PtCu nanohemicubes, and PtPdCu nanocubes were prepared successfully on the surface of GO in molten salt. Introduction of GO as the stabilizer in molten salt proves a new approach in synthesis of Pt-based nanocrystals with controlled morphologies.
研究领域:
材料科学
·
纳米技术
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Fangfang Fan,Du-Hong Chen,Linjuan Yang,Jiuhui Qi,Youjun Fan,Yixuan Wang,Wei Chen
The controllable synthesis of 1-dimensional (1D) multi-metal Pt-based alloys, with enhanced electro-chemical properties remains a challenge, despite the wide application of Pt-based catalysts in fuel cells and in the hydrogen evolution reaction (HER). Herein, we fabricate PtCuFe alloy nanochains (NCs) that have a tunable composition by flexibly adjusting the molar ratios of the metal precursors. It was found that Cu 2+ is key in the formation of 1D NCs, as confirmed by transmission electron microscopy characterizations. In addition, the alloyed Fe can further increase the content of the metallic state of Cu in the PtCuFe NCs. The as-prepared PtCuFe NCs exhibited higher catalytic activity and stability than those of the Pt nanoparticles (NPs), PtFe NPs, and PtCu NCs, for the methanol oxidation reaction (MOR) and HER . Additionally, the composition-performance relationship of PtCu x Fe y NCs toward the MOR and HER were investigated. The hybrid density functional theory calculation and analysis showed that the 1D PtCuFe NCs have a lower lowest unoccupied molecular orbital (LUMO) than those of the 2- and 3-dimensional PtCuFe, verifying that the 1D PtCuFe NCs exhibit the highest activity for the MOR. This work has established a new method for the controllable synthesis of multi-metal Pt-based NCs/alloy catalysts and their subsequent applications in other electro-catalytic reactions.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Nano
·
2023
·
IF 17.1
Shuai Zhang,Leilei Yin,Siyuan Wang,Jin-Cheng Liu,Yabin Zhang,Yongqing Wen,Qian Zhang,Yaping Du
Rare earth (RE) elements possess electronic configurations that can provide additional pathways for tailoring the electronic structures of active elements through alloying, making it an important area of exploration in electrocatalysis. However, the large negative redox potential between RE and Pt has hindered the development of RE nanoalloys. In this study, a solid-phase synthesis strategy was employed to synthesize ternary Pt3–xIrxSc nanoparticles (NPs). By leveraging the electronegativity difference between Pt (2.28), Ir (2.20), and Sc (1.36), a charge-balance strategy was implemented to stabilize and enhance the catalytic performance of the alloy. The electron transfer from Sc to Pt/Ir results in the latter being negatively charged, and the Ir modifies the electron density of Pt, enabling favorable adsorption of active H species during the hydrogen evolution reaction (HER). Pt2IrSc exhibits enhanced HER activity at all pH values, achieving low overpotentials at 10 mA cm–2 of only 13, 18, and 25 mV in 0.5 M H2SO4, 1 M PBS, and 1 M KOH, respectively. This electrocatalyst also exhibits robust electrocatalytic stability even after 20,000 cycles. This work represents an application of the charge balance strategy to RE nanoalloys, and it is expected to inspire the design and synthesis of highly reactive RE nanoalloys.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Wendi Yi,Ruohan Yu,Haoqing Jiang,Jinsong Wu,Gary J. Cheng
The formation of high-density atomic metal layers on 2D materials enhances catalytic device development by providing a large surface area, precise control over active sites, and enhanced reactivity. Here, pulsed laser-induced chemical solid-phase deposition (LCSD) is introduced for achieving high-density atomic metal layers. By leveraging high-density plasma generated via pulsed nanosecond laser irradiation of thin salt layers on 2D materials, atomic-scale metals are deposited onto abundant nucleation sites, creating dense atomic-metal layers. This study engineers layered double hydroxide (LDH) materials layered with atomic platinum-based alloys, exhibiting exceptional catalytic activity for overall water splitting. LDH's excellent oxygen evolution performance combined with remarkable advances in hydrogen evolution catalysis are achieved. Introducing a second element improves Pt layer dispersion and uniformity, resulting in extraordinary Pt distribution density and minimal overpotential. The LDH and Pt-metal combination creates powerful synergistic effects, significantly enhancing catalytic performance and enabling superior bifunctional catalysts for water splitting. LCSD effectively fabricates stable nanocomposites designed for electrocatalytic applications, leveraging unique structures of atom-scale metal-supported composite 2D materials, enhancing overall electrocatalytic performance. This breakthrough impacts energy conversion and environmental protection, broadening electrocatalysis and revolutionizing atom-scale metal-supported composite 2D materials. Its practical applications span various areas, contributing to sustainable energy solutions and environmental preservation.
研究领域:
材料科学
·
电催化
·
能源转换
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Liu Xuan,Wang Yuhan,He Hu,Zhao Zhonglong,Luo Xuan,Zhang Siyang,Lu Gang,Su Dong,Wang Yucheng,Huang Yunhui,Li Qing
The long-standing challenges facing Pt-based alloy catalysts in oxygen reduction reactions (ORRs) are rapid oxidation and loss of transition metal/Pt in proton exchange membrane fuel cells (PEMFCs). In this work, we report a concept of “covalentization” in intermetallic L1 0 -PtMM’ (M = Fe, Co, Ni and M’ = one of the 4 th -period elements (from Ti to Ge)) alloys to enhance their electrochemical stability. Specifically, the formation of a quasi-covalent bond network in L1 0 -PtMM’ due to the less occupied antibonding states induced by high d -band positions of M’ elements (e.g., Ti, V, Cr) enhances atomic bond order and strength, diminishing Co anodic dissolution via strengthened Pt/Co-M’ bonds and reducing Co cathodic corrosion by inhibiting Pt oxidation through an electron buffering effect. The developed L1 0 -PtCoCr/C catalysts show a high mass activity (MA = 1.27 A mg Pt −1 ) and rated power (16.5 W mg Pt −1 ) in PEMFCs at a low total Pt loading of 0.075 mg Pt cm −2 . The catalysts also exhibit high electrochemical stability with ~3% and 5% loss of MA and rated power after 30,000 accelerated durability testing cycles and projects a lifetime of about 42,000 hours.
研究领域:
材料科学
·
能源工程
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Xuyuan Nie,Guang Li,Linzhe Lü,Lifei Ji,Jian Yang,Yan-Xia Jiang,Binwei Zhang,Zidong Wei,Shi-Gang Sun
The surface electron structure of metal catalysts plays a crucial role in their catalytic performance. Nevertheless, developing simple and reliable methods to evaluate this structure remains challenging. Here, we introduce an electrochemical in situ Fourier transform infrared spectroscopy (FTIRS) CO adsorption probe method to study the surface structure of Pt-based alloy catalysts. Combined with high-angle annular dark-field scanning transmission electron microscopy, X-ray photoelectron spectroscopy, and the in situ FTIRS CO-probe method, our study demonstrated that the red/blueshift of COad wavenumbers could be attributed to the modifications in the surface Pt electronic structure, resulting in a shift of the d-band center for Pt. This would enhance the d-π* feedback effect between Pt and CO and result in the redshifts of the CO adsorption peaks. This phenomenon can also be observed in transition metal–nitrogen–carbon catalysts, further proving the universality of the in situ FTIRS CO-probe method.
研究领域:
催化化学
·
材料科学
✓ 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）