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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Templated-Assisted Synthesis of Structurally Ordered Intermetallic Pt3Co with Ultralow Loading Supported on 3D Porous Carbon for Oxygen Reduction Reaction

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
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Single-atom Pt-CeO2/Co3O4 catalyst with ultra-low Pt loading and high performance for toluene removal

Huihui Shi,Peixin Yang,Lu Huang,Yali Wu,Duohuan Yu,Hangfei Wu,Yunhuai Zhang,Peng Xiao

The design and manufacture of high activity and thermal stability catalysts with minimal precious metal loading is essential for deep degradation of volatile organic compounds (VOCs). In this paper, a novel single-atom Pt-CeO 2 /Co 3 O 4 catalyst with ultra-low Pt loading capacity (0.06 wt%, denoted as 0.06Pt-SA) was fabricated via one-step co-precipitation method. The 0.06Pt-SA exhibited excellent toluene degradation activity of T 90  = 169 °C, matched with the nanoparticle Pt-supported CeO 2 /Co 3 O 4 catalyst with more than six times higher Pt loading (0.41 wt%, denoted as 0.41Pt-NP). Moreover, the ultra-long durability (toluene conversion remains 99% after 120 h stability test) and excellent toluene degradation ability in a wide space speed range of 0.06Pt-SA were superior to that of 0.41Pt-NP catalyst. The excellent performance was derived from the strong metal-support interaction (SMSI) between the single atomic Pt and the carrier, which induced more Pt 0 and Ce 3+ for oxygen activation and more Co 3+ for toluene removal. The in situ   diffuse reflectance infrared spectroscopy (DRIFTS) experiments confirmed that the conversion of intermediates was accelerated in the reaction process, thereby promoting the toluene degradation. Our results should inspire the exploitation of noble single-atomic modification strategy for developing the low cost and high performance VOCs catalyst.

研究领域: 催化化学 · 环境科学 · 材料科学
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ELECTROCHIMICA ACTA · 2023 · IF 6.6

The underlying mechanism trade-off between particle proximity effect and low-Pt loading for oxygen reduction and methanol oxidation reaction activity

Jiarun Cheng,Chaojie Lyu,Gang Dong,Yongqiang Liu,Yue Hu,Bin Han,Dongsheng Geng,Dongjie Zhao

Highly efficient and stable Pt-based electrocatalysts have broad application prospects in fuel cells, among which, Pt loading accompanied with particle size, interparticle distance (ipd), and interaction with support are identified as key contributors for high activity and selectivity. Herein, we have developed the nitrogen-doped graphite-like carbon sheets supporting low-Pt loading (Pt@N-GC) with uniform size and controllable ipd, and disentangled the main effect of ipd on oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activity. The optimal 5.0 wt% low-Pt loading results in more abundant Pt sites and lower ipd, which leads to the higher surface reactivity by proximity effect , and 2e − pathway can be hindered by strongly resorbing and reducing H 2 O 2 to promote 4e − pathway towards ORR . Simultaneously, the 5.0 wt% Pt@N-GC can effectively improve the MOR activity, enhance the adsorption of -OH group under the appropriate ipd, so as to promote the instantaneous oxidation of CO and enhance the tolerance, and accelerate the oxidative dehydrogenation of methanol. Benefiting by the synergistic effect of Pt nanoparticles and N-GC support, all Pt@N-GCs exhibit bifunctional electrocatalytic activity and durability. We believe the gained trade-off of the loading and proximity effect of Pt, and its influence on catalytic activity and selectivity contributes to design more promising low-Pt loading bifunctional catalysts for fuel cell.

研究领域: 材料科学 · 电化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2024 · IF 4.1

Co-doped hollow nanospheres with low Pt loading for electrocatalytic oxygen reduction and zinc-air batteries

Lijing Yang,Junhong Ma,Yuemei Liu,Chaoyun Ma,Xue Yu,Ziyang Meng

Preparing high-performance catalysts for oxygen reduction reaction (ORR) with low Pt loading is crucial to promote the development of clean energy storage devices such as metal air batteries. Herein, Co/ N -HCMs support material with isolated Co atoms and hollow flower-like structure could be prepared by a self-sacrificing template strategy. Co/ N -HCMs are then used to anchor Pt to obtain PtCo/ N -HCMs catalyst with low Pt loading. Thanks to its improved specific surface area, hierarchical porous structure, and reinforced metal-support interactions, the obtained PtCo/ N -HCMs deliver high onset potential of 0.99 V and half-wave potential of 0.82 V, and an excellent durability. When used as air cathode catalyst, PtCo/ N -HCMs-based Zinc-air battery (ZAB) exhibits a power density of up to 202 mW cm −2 , which is significantly better than ZAB assembled with commercial Pt/C. This study provides an effective strategy for preparing high-performance electrocatalysts with low precious metal content for use as the cathode of metal-air batteries.

研究领域: 材料科学 · 电化学 · 能源存储与转换
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ACS Applied Energy Materials · 2021 · IF 6.024

Porous Pt-Ni Nanobelt Arrays with Superior Performance in H2/Air Atmosphere for Proton Exchange Membrane Fuel Cells

Dewei Yao,Hongmei Yu,Wei Song,Xueqiang Gao,Xinye Sun,Guang Jiang,Jinkai Hao,Zhigang Shao

To reduce cost and energy consumption of fuel cell vehicles, constructing membrane electrode assemblies (MEAs) with low Pt loading and outstanding performance at low relative humidity (RH) conditions is reported. A catalyst layer based on porous Pt–Ni nanobelt arrays was prepared, in which the strained catalyst enhanced the catalytic activity and the oriented nanobelt array structure provided convenient mass transport channels. The porous Pt–Ni nanobelt arrays were prepared by the magnetron sputtering of Pt and Ni on a sacrificed template and then washed with acid. Consequently, the catalyst layer based on the porous Pt–Ni nanobelt arrays exhibited superior fuel cell performance in H2/air conditions and RH 40%. The performance of the MEA with porous Pt–Ni nanobelt arrays reach 366.6 and 597.6 mW cm–2 with Pt loadings of 36.5 μg cm–2/36.5 μg cm–2 and 108.9 μg cm–2/108.9 μg cm–2 at the cathode/anode, respectively. A conventional CCM with the Pt loading of 100 μg cm–2/200 μg cm–2 at the cathode/anode served as the benchmark, and the cell performance was 230.5 mW cm–2. Apart from that, the Pt nanobelt arrays without a porous structure (100.8 g cmPt–2/100.8 μg cmPt–2) serving as another benchmark achieved a performance of 504.7 mW cm–2. The superior performance of the porous Pt–Ni nanobelt arrays is attributed to the convenient mass transport pathway and the high activity of the porous Pt–Ni nanobelt.

CAS / MDL: 10026-22-9 57-13-6
研究领域: 材料科学 · 能源技术
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Metal-support interaction promoted multifunctional electrocatalysis on PtCo/NC with ultralow Pt loading for oxygen reduction reaction and zinc-air battery

Manting Zhang,Tingting Zhou,Danil Bukhvalov,Fengyan Han,Caiqin Wang,Xiaofei Yang

Tri-functional PtCo/NC nanocatalysts were assembled via in-situ integration with ultralow Pt loading supported on ZIF-67 derived porous carbon material, and used as electrocatalysts for oxygen reduction reaction (ORR), ethanol oxidation reaction (EOR), hydrogen evolution reaction (HER). Detailedly, PtCo-3/NC with ultralow Pt loading (1 wt%) exhibits the halfwave potential of 0.877 V for ORR in acidic media and considerable current density for both ORR and EOR at 0.85 V, and low overpotential (η 10 =10 mV) for HER. The as-assembled zinc-air batteries (ZABs) based on PtCo/NC have higher power density than Pt/C based ZABs. DFT calculation reveals the strong metal-support interactions (MSI) in PtCo/NC, which leads to the change of electronic state, redistribution of charge density and optimization of free energy , allowing it to present greater performances than Pt/C. This work highlights the possibility of using it as highly effective electrode catalysts with ultralow Pt loading in fuel cells and metal-air battery.

CAS / MDL: 10026-22-9 10025-99-7
研究领域: 材料科学 · 电化学 · 能源科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

Free-standing and ionomer-free 3D platinum nanotrough fiber network electrode for proton exchange membrane fuel cells

Manman Qi,Yachao Zeng,Ming Hou,Yong Gou,Wei Song,Haiping Chen,Gang Wu,Zhenghao Jia,Yanyan Gao,Hongjie Zhang,Zhigang Shao

Herein, a nanotrough-like catalyst layer (NTCL) with low Pt loading and enhanced durability was developed directly as the cathode for proton-exchange membrane fuel cells (PEMFCs). Benefiting from the biomimetic architecture and ultrathin thickness, the mass transport of reactants and water management in the cathode are significantly enhanced. A peak power density of 0.936 W cm −2 is achieved with a Pt loading of 42 μg cm −2 in the cathode. Besides, the in-situ observation of water formation on the NTCL by the environmental scanning electron microscopy (ESEM) verified the efficient water management. Importantly, the Pt NTCL cathode is far more stable than the conventional electrode during the accelerated stress tests. The enhanced durability may be attributed to a self-healing mechanism, which involves Pt dissolution and re-deposition, endowing the NTCL with outstanding robustness. This work highlights a new approach to preparing and understanding nanostructured Pt electrodes with enhanced performance and durability for PEMFCs.

研究领域: 电化学 · 纳米材料 · 能源材料 · 燃料电池 · 电催化 · 表面科学 · 环境扫描电镜
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2018 · IF 5.091

Confining nano-sized platinum in nitrogen doped ordered mesoporous carbon: An effective approach toward efficient and robust hydrogen evolution electrocatalyst

Yaqing Yin,Tingting Liu,Dan Liu,Zhao Wang,Qibo Deng,Deyu Qu,Zhizhong Xie,Haolin Tang,Junsheng Li

Despite recent progress in the development of earth abundant electrochemical catalyst for hydrogen evolution reaction (HER), Pt based materials still stand as the state of the art HER catalyst. Due to the high cost of Pt, it is desirable to increase the utilization efficiency of Pt in practical HER process to a realize cost effective hydrogen production . Herein, we repot a novel nitrogen doped ordered mesoporous carbon supported Pt (Pt@NOMC-A) catalyst with a low Pt loading of 7.2 wt% and show that the synergy between Pt nanoparticles and carbon support, as well as the physical confinement offered by the carbon support enhance the electrochemical performance of the novel catalyst. Pt@NOMC-A exhibits a low HER overpotential comparable with commercial 20 wt% Pt/C catalyst under acidic, neutral and alkaline condition. Furthermore, Pt@NOMC-A shows a superior electrochemical stability under working conditions suppressing that of commercial Pt/C catalyst.

CAS / MDL: 56-87-1
研究领域: 材料科学 · 电化学 · 能源材料
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Synergistic Effect of Electrocatalyst for Enhanced Oxygen Reduction Reaction: Low Pt-Loaded CuPt Alloy Nanoparticles Supported on N-Doped Hierarchical Porous Carbon

Min Li,Feng Liu,Yongming Zhang

It is challenging to synthesize oxygen reduction reaction (ORR) electrocatalysts that are highly efficient, affordable, and stable for use in proton exchange membrane fuel cells. To address this challenge, we developed a low platinum-loading (only 6.68% wt) ORR catalyst (PtCu1-NC), comprising CuPt nanoparticles (average size: 1.51 nm) supported on the N-doped carbon substrates. PtCu1-NC possesses a high specific surface area of 662 m2 g–1 and a hierarchical porous structure, facilitating efficient mass transfer. The synergistic effect from introduced copper and the electron effect from nitrogen modify the electronic structure of platinum, effectively accelerating the ORR reaction and enhancing stability. Density functional theory calculations demonstrate the catalytic mechanism and further verify the synergistic effect. Electrochemical assessments indicate that PtCu1-NC exhibits specific activity and mass activity 5.3 and 5.6 times higher, respectively, than commercial Pt/C. The half-wave potential is 27 mV more positive than that of commercial Pt/C. The electrochemical active surface area value is 104.3 m2 g–1, surpassing that of Pt/C. Approximately 78% of current is retained after 10,000 s chronoamperometry measurement. These results highlight the effectiveness of alloying in improving the catalyst performance.

研究领域: 材料科学 · 电化学 · 催化 · 能源材料
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Ultralow-Loading Platinum Catalysts Anchored by Lacunary POMs Proton Pumps for Proton Exchange Membrane Water Electrolysis

Huawei Shen,Yichao Huang,Pengcheng Zhao,Ruili Gao,Zheyu Wei,Xiaohui Gao,Meihong Liao,Weijiang Dai,Xuezhao Liu,Desheng Sui,Jun Liu,Shangqian Zhu,Yongge Wei

Developing highly active and stable electrocatalysts for practical proton exchange membrane water electrolyzers (PEMWEs) operating at industry-relevant current densities remains a significant challenge. In particular, the hydrogen evolution reaction (HER) at ampere-level current densities leads to the rapid consumption of interfacial protons, resulting in sluggish kinetics. Herein, a strategy is proposed to reduce the proton transfer energy barriers and improve the HER kinetics at high current densities by anchoring tri-lacunary Keggin-type polyoxometalates (POMs) on Pt. The lacunary POMs clusters function as proton pumps, increasing the connectivity of hydrogen bond networks and enabling proton transfer via a proton-coupled electron transfer mechanism. In addition, an unconventional Tafel step mediated by short-pathway hydrogen spillover from POMs clusters to Pt active sites is also created. As a result, an ultra-high mass activity of 782.94 A·mg Pt −1 and remarkable durability over 6000 h at a current density of 2000 mA·cm −2 can be simultaneously achieved in a practical PEMWE with an ultralow Pt loading mass of 4.2 µg Pt ·cm −2 . The strategy provides new opportunities in developing next-generation low-Pt electrocatalysts for PEMWE applications.

研究领域: 电催化 · 能量转换 · 水电解 · 材料科学 · 催化剂设计 · 可再生能源
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