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ACS Catalysis · 2019 · IF 12.221

One-Nanometer-Thick Pt3Ni Bimetallic Alloy Nanowires Advanced Oxygen Reduction Reaction: Integrating Multiple Advantages into One Catalyst

Mingxing Gong,Zhiping Deng,Dongdong Xiao,Lili Han,Tonghui Zhao,Yun Lu,Tao Shen,Xupo Liu,Ruoqian Lin,Ting Huang,Guangwen Zhou,Huolin Xin,Deli Wang

Developing highly active as well as durable oxygen reduction reaction (ORR) electrocatalysts are still imperative for clean and efficient energy conversion device, such as fuel cells and metal-air battery. For this purpose and maximize the utilization of noble Pt, we present here a facile, yet scalable strategy for the high-precise synthesis of 1-nm-thick Pt3Ni bimetallic alloy nanowires (Pt3Ni BANWs). The seed-mediated growth mechanism of Pt3Ni BANWs was identified subsequently. As expected, the Pt3Ni BANWs delivered enhanced mass activity (0.546 A mgPt–1, exceeding the 2020 target of DOE) in comparison to Pt nanowires assembly (Pt NWA, 0.098 A mgPt–1) and Pt/C (Pt, 0.135 A mgPt–1), because of the rational integration of multiple compositional and structural advantages. Moreover, the Pt3Ni BANWs displayed enhanced durability (37% MA retention) than Pt NWA and Pt after 50 000 potential cycles. All these results indicate that the ultrathin Pt3Ni BANWs are potential candidates for catalyzing ORR with acceptable activity and durability. The present work could not only provide a facile strategy but also a general guidance for the design of superb performance Pt-based nanowire catalysts for ORR.

CAS / MDL: 64-17-5 68-12-2 107-21-1
研究领域: 材料科学 · 电化学 · 能源转换技术
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Molten-Salt Motivated MXene-Based Heterostructure Activate Pt Clusters for Hydrogen Evolution Reaction

Xin Sun,Jing Yu,Yan Zhang,Qi Liu,Rongrong Chen,Jingyuan Liu,Jiahui Zhu,Jun Wang

Atomic clusters exhibit superior performance in heterogeneous catalysis due to their unique electronic states and highly exposed active surfaces. Nevertheless, significant challenges persist in achieving the precise and efficient synthesis of atomic clusters while preventing undesirable formation of coexisting species, particularly nanoparticles. Herein, a one-step in situ phase transition engineering strategy is reported for the synthesis of atomic platinum clusters by vapor deposition on Ti 3 C 2 Cl 2 MXene and TiC heterogeneous interface (Pt-MXene/TiC) in molten salt, where Pt clusters can be acquired over a slight amount of Pt contents (0.298 wt.%). The strongly polarized molten salt induces the desired confinement of atomic-scale Pt clusters. The construction of heterogeneous interfaces enhances the local electric field and accelerates the electron transfer between Pt and the substrate. As a result, Pt-MXene/TiC-950 exhibits an exceptional increase in mass activity and turnover frequency (TOF) for hydrogen evolution reaction (HER) at 49.4 and 46.7 folds of 10% commercial Pt/C. Further theoretical calculations elucidate that the Pt species in Pt-MXene/TiC-950 possess moderate d-band center, which enables optimized selectivity and activity for intermediates adsorption in HER process. This work provides some guidelines for leveraging molten salt and heterostructure to enhance the precision and synthesis efficiency of atomic clusters.

CAS / MDL: 7646-85-7
研究领域: 材料科学 · 催化化学
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ACS Catalysis · 2018 · IF 11.384

Hexapod PtRuCu Nanocrystalline Alloy for Highly Efficient and Stable Methanol Oxidation

Shengfeng Xue,Wentao Deng,Fang Yang,Jinlong Yang,Ibrahim Saana Amiinu,Daping He,Haolin Tang,Shichun Mu

A hexapod PtRuCu nanocrystalline alloy material is successfully fabricated by a facile approach based on Stranski–Krastanov growth and galvanic replacement and used as an efficient catalyst for direct methanol fuel cells (DFMCs). Because of the synergetic effect of metallic elements in the methanol oxidation, the activity and durability of the prepared PtRuCu/C catalyst is significantly enhanced. It has a mass activity of 1.35 A mgPt–1 and a specific activity of 3.92 mA cm–2, which are 3.8 and 8.2 times higher than those of Pt/C, respectively. Its mass activity only decreases 27% after 800 CV cycles compared with Pt/C (60% decline), indicating the admirable stability of the PtRuCu catalyst.

研究领域: 材料科学 · 能源化学
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 20 ·12196-12202 · IF 12.732

Ru single atoms and nanoclusters on highly porous N-doped carbon as a hydrogen evolution catalyst in alkaline solutions with ultrahigh mass activity and turnover frequency

Yijun Li,Huijing Liu,Bing Li,Zhenzhen Yang,Zhenguo Guo,Jian-Bo He,Jianhui Xie,Tai-Chu Lau

Electrocatalytic water splitting is one of the most desirable ways to produce hydrogen, which is a clean and sustainable energy source. Improving the formation and the exposure of active sites is a key issue in the design of cost-effective and efficient metal-based electrocatalysts, especially for noble metals, in order to cut down the metal content and improve the mass activity of the metals, while maintaining high catalytic activity. Herein, we report a high-performance Ru-based electrocatalyst consisting of Ru single atoms and Ru nanoclusters encapsulated in highly porous N-doped carbon with abundant hierarchical pores (Ru/p-NC). Remarkably, Ru/p-NC shows excellent HER activity in 1.0 M KOH with a low overpotential of 10 mV at 10 mA cm−2, a small Tafel slope of 17 mV dec−1 as well as good durability for 24 h, outperforming commercial Pt/C and Ru/C catalysts. More importantly, the mass activity and turnover frequency (based on Ru loading) of Ru/p-NC are ultrahigh owing to the low loading of Ru, which are 17 A mgRu−1 and 8.9 H2 s−1, respectively, at a very low overpotential of 25 mV. Experimental results indicate that the porous N-doped carbon support not only leads to exposed active sites but also interacts strongly with the Ru moieties. In addition, it tunes the electronic structure of the catalyst, boosts the stability as well as facilitates mass transport and charge transfer kinetics. This work provides a new route for the synthesis of metal-based porous N-doped carbon hybrid electrocatalysts with abundant exposed active sites and strong metal-support interaction for energy conversion.

研究领域: 材料科学 · 电化学 · 能源转换
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2020 · IF 3.807

Ultrathin PtCo nanorod assemblies with self-optimized surface for oxygen reduction reaction

Shuqi Hu,Zhen Wang,Hongling Chen,Shuangbao Wang,Xianguo Li,Xinyi Zhang,Pei Kang Shen

Controllable synthesis of Pt-based materials at the nanoscale can efficiently tailor their electrocatalytic performance, enabling enhancement in both activity and durability. Herein, we report the synthesis of ultrathin PtCo nanorod assemblies (NRAs) terminated with high index facets through a grain-boundary corrosion approach. Atomic insight reveals that grain boundaries and other defects are formed in PtCo nanowire assemblies (NWAs) during the hydrothermal reaction . With a further increase in reaction time, selective dissolution at these sites generated PtCo NRAs composed of shorter nanorod assemblies with larger surface areas and high index facets termination. The carbon-supported catalyst of PtCo NRAs exhibits high mass activity of 0.914 A/mg Pt at 0.9 V vs RHE for ORR , 2.4 times higher than those of the smooth PtCo NWAs (0.377 A/mg Pt ), 5.7 times higher than those of the commercial Pt/C (0.161 A/mg Pt ). Most significantly, the PtCo NRAs show high stability with about 25.6% loss of mass activity after 10,000 cycles, while only 22.3% loss of mass activity from 10,000 cycles to 50,000 cycles of accelerated durability test. The high durability is mainly attributed to the jagged surface resulted from the surface reconstruction of PtCo NRAs during the electrochemical process. This self-optimization phenomenon may lead to a new effective long-life electrocatalyst .

研究领域: 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

Worm-like PtCux alloys oriented by pyrolyzed alginic acid sodium with high performance in methanol electrooxidation

Huimin Li,Zheng Si,Jinli Zhang,Yan Fu,Wei Li

Worm-like PtCu x alloys were synthesized through the co-reduction of H 2 PtCl 6 and CuCl 2 in ethylene glycol under the orientation of pyrolyzed alginic acid sodium (PA), in order to disclose the growth mechanism of different metallic compounds. Through the characterizations of FTIR, Raman, XRD , XPS , TEM , etc., it illustrates that with the orientation of oxygen-containing functional groups in the support PA, the preferentially reduced Pt clusters accelerate the formation of metallic Cu clusters and then worm-like bimetallic PtCu x alloys are generated with plenty of surface defects . The synthesized PtCu 3 /PA exhibits the highest content of metallic Pt 0 (67.11 at%), the average width about 2.19 nm, the lattice strain of −1.18%, as well as the excellent performance for methanol electrooxidation . It has the best CO tolerance ability and the optimal mass activity of 1.922 A mg Pt −1 , which is more than four times of the commercial Pt/C. This work discloses an intriguing growth pathway of PtCu x nanoparticles but also a facile route to synthesize bimetallic alloys with more electrocatalytic activity .

研究领域: 材料科学 · 电化学
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CATALYSIS TODAY · 2022 · IF 6.562

Engineering ultrafine Ir nanocrystals for electrochemical hydrogen evolution with highly superior mass activity

Hui Li,Hehe Wei,Longtao Zhang,Zixiang Su,Xueqing Gong

Highly active and durable noble metal-based catalysts for electrochemical hydrogen evolution are crucial for clean and renewable energy production, however, low abundance and high price hinder their development at industrial scale. Herein, we synthesized carbon-supported ultrafine iridium nanoparticles (Ir NPs/C) catalyst via solvothermal method which achieved ultralow overpotentials of 13 and 57 mV at the current density of 10 and 100 mA cm −2 for hydrogen evolution reaction (HER) in acidic media, respectively. The prepared Ir NPs/C catalyst also exhibited ultrahigh mass activity of 44.5 A mg −1 at the overpotential of 40 mV and outstanding long-term stability in HER performance for 12 h, remarkably superior to state-of-the-art commercial Pt/C catalyst (3.3 A mg −1 , fast decay) and commercial Ir/C catalyst (1.2 A mg −1 ). Furthermore, it possessed activities toward oxygen evolution reaction (OER) and overall water splitting. This work demonstrates evenly dispersed fine Ir NPs/C catalyst can facilitate highly efficient HER and provides inspiration for rational design of advanced electrocatalysts.

研究领域: 材料科学 · 能源化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Twin Boundary-Regulated Platinum–Yttrium Elemental Distributions for Boosting Electrochemical Alcohol Oxidation

Zhen He,Chen Ma,Huangxu Li,Chengming Wang,Lingwen Liao

Metastable crystal defects endow nanocrystals with optimized electronic configurations and remarkable electrocatalytic properties. Nevertheless, how the crystal defects, such as twin boundaries, regulate the nucleation and growth of multimetallic heterostructures requires further study. Herein, platinum–yttrium (PtY) alloys with a metastable twin structure were fabricated by overgrowth on Au nanoparticles, resulting in the formation of Au@PtY multibranched nanodendrites (Au46Pt40Y14). The branched Au@PtY nanoparticle exhibits a Y-rich twin structure on the surface, as affirmed by both experimental investigation and theoretical calculation. Impressively, branched Au@PtY nanoparticles demonstrate superior mass activity and stability toward the alcohol oxidation reaction, compared to core–shell Au@PtY nanoparticles (Au67Pt25Y8), PtY nanodendrites (Pt73Y27), and commercial Pt/C catalysts. Density functional theory calculations, together with operando infrared reflection absorption spectroscopy, suggest that the superior electrochemical characteristics could be ascribed to the Y-rich twin on the surface. This work opens the way for the rational design of heterometallic nanostructures with crystal defects for catalytic applications.

研究领域: 材料科学 · 电催化
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Journal of Materials Chemistry A · 2017 ·Vol. 5 ·期 4 ·1623-1628 · IF 8.867

Rh–Ag–Si ternary composites: highly active hydrogen evolution electrocatalysts over Pt–Ag–Si

Binbin Jiang,Yuyang Sun,Fan Liao,Wen Shen,Haiping Lin,Hui Wang,Mingwang Shao

Hydrogen production with the aid of electrocatalysis is a critical component for several developing clean-energy technologies. Such a renewable energy depends heavily on the choice of cheap and efficient catalysts for hydrogen evolution, which has still been a challenge until now. In this work, the theoretical calculation indicates that Rh–Ag–Si ternary catalysts exhibit more active hydrogen evolution performance than Pt–Ag–Si because the migration activation energies of H atoms from Rh(111) to Si are lower than those from Pt(111) to Si via the Ag surface. This simulation was confirmed by the experimental results: Rh–Ag/SiNW (or Pt–Ag/SiNW) catalysts were prepared by directly reducing Rh (or Pt) and Ag ions with Si–H bonds. The Rh–Ag/SiNW-2 with the optimal mass ratio of 2.3 : 23.4 : 74.3 (Rh : Ag : Si) exhibited a lower Tafel slope (51 mV dec−1) and a larger exchange current density (87.1 × 10−6 A cm−2) than the Pt–Ag/SiNW. In addition, the mass activity of Rh–Ag/SiNW-2 at an overpotential of 0.2 V (11.5 mA μgRh−1) is 12.0, 5.0 and 3.3 fold higher than that of Rh–Ag (0.96 mA μgRh−1), Pt–Ag/SiNW (2.3 mA μgPt−1) and 40 wt% Pt/C (3.5 mA μgPt−1) catalysts, respectively. Moreover, the Rh–Ag/SiNW nanocatalysts had good stability in acidic media. The results presented herein may offer a novel and effective methodology for the designing of cost-efficient and environmentally friendly catalysts for electrochemical fields.

CAS / MDL: 18497-13-7 13569-65-8
研究领域: 材料科学 · 能源化学
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CATALYSIS TODAY · 2018 · IF 4.667

High Pt utilization efficiency of electrocatalysts for oxygen reduction reaction in alkaline media

Ningqiang Zhang,Lingcong Li,Ya Chu,Lirong Zheng,Shaorui Sun,Guizhen Zhang,Hong He,Jinsheng Zhao

Electrocatalyst for oxygen-reduction reaction (ORR) is crucial for metal-air batteries, in which Pt-based materials are the benchmark catalysts for ORR. However, the high cost and limited supplies of Pt limit its broad use in commercial applications. Designing highly efficient Pt electrocatalysts can reduce material cost and enable commercial success for a wide variety of electrochemical technologies. Herein, we prepared Pt/MnO x and Pt/MnO electrocatalysts via deposition–precipitation and H 2 –reduction approaches. The Pt mass activities towards the ORR at 0.7 V for the Pt/MnO x , and Pt/MnO catalysts were 4.0 and 3.7 A mg Pt −1 , respectively, which were 20, and 18.5 times as commercial 20% Pt/C catalyst. The transferred electron numbers (n) were 3.6 and 4.0 for Pt/MnO x and Pt/MnO, respectively. Moreover, Pt/MnO catalyst exhibited a good ORR stability after 500 cycles compared to Pt/MnO x catalyst in 0.1 M KOH.

CAS / MDL: 67-63-0
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Trace Ru-tuned NiO/CNT electrocatalysts outperform benchmark Pt for alkaline hydrogen evolution with superior mass activity

Yanjun Chen,Yiyang Lee,Wei Chu,Jing Li

The exploitation of highly active and durable electrocatalysts that can replace high-cost Pt/C for hydrogen evolution reaction (HER) is urgently required. The challenge lies in diminishing the usage of noble metals without sacrificing HER activity. In this work, trace Ru-doped transition metal oxides (TMOs) nanoparticles (∼7 nm) with high dispersion loaded by the carbon nanotubes (CNTs) were developed. Specifically, Ru-NiO/CNTs with a low Ru content of 0.94 wt% exhibits excellent alkaline HER activity with the low overpotential of 19 mV and 98 mV to achieve the current density of 10 mA·cm −2 and 100 mA·cm −2 , respectively, outperforming Ru/CNTs counterpart and most previously Ru-based nanocatalysts. Notably, the mass activity (1.83 A·mg Ru -1 ) and price activity (301.51 A·dollar -1 ) of Ru-NiO/CNTs are separately more than 7 times and 18 times higher than that of the commercial 20% Pt/C benchmark. Moreover, the catalyst can operate without activity decay after 100 h long-term stability test. DFT calculation reveals that the synergy effects are originated from (i) the accelerated adsorption and dissociation of H 2 O by Ru, and (ii) the optimized electronic structure of Ni that tunes the H* adsorption/desorption. Furthermore, we discover that Ru-promoted HER activity shows a metal-dependent relationship (Ni ≈ Cu > Mn > Co > Fe), which can use binding energy shift (ΔE) as a highly correlated descriptor. This work may provide an insightful understanding of Ru dopant for enhanced HER activity.

CAS / MDL: 10026-22-9 10049-08-8
研究领域: 材料科学 · 电化学 · 催化科学
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Journal of the American Chemical Society · 2022 · IF 16.383

Ru Colloidosome Catalysts for the Hydrogen Oxidation Reaction in Alkaline Media

Xiaodong Yang,Bo Ouyang,Peiqi Shen,Yiqiang Sun,Yisong Yang,Yanan Gao,Erjun Kan,Cuncheng Li,Kun Xu,Yi Xie

Developing efficient hydrogen oxidation reaction (HOR) electrocatalysts in alkaline media is of great significance for anion exchange membrane fuel cells. Herein, we report the synthesis of hollow colloidosomes composed of Ru nanocrystals based on a novel gas/liquid interface self-assembly strategy. Structural characterizations reveal that much defects are present in the building block (Ru nanocrystals) of Ru colloidosomes. Theoretical calculations suggest that the defects in the Ru structure can optimize the adsorption binding energy of reaction intermediates for the HOR. Benefiting from the assembled colloidosome and optimized electronic structure, the Ru colloidosomes exhibit remarkable HOR catalytic performance in alkaline media with a mass activity higher than that of benchmark Pt/C. Our work may shed new light on the rational design of advanced electrocatalysts with an assembled structure for energy-related applications.

研究领域: 材料科学 · 电化学
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