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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

ZIF-67-derived Co nanoparticles embedded in N-doped porous carbon composite interconnected by MWCNTs as highly efficient ORR electrocatalysts for a flexible direct formate fuel cell

Zhenfei Liu,Dingding Ye,Xun Zhu,Shaolong Wang,Yanan Zou,Linghan Lan,Rong Chen,Yang Yang,Qiang Liao

Non-precious metal materials are considered as the most promising catalysts for oxygen reduction reaction (ORR) due to their high catalytic activity, low cost, superior stability as well as good electrocatalytic selectivity. Here, in situ encapsulation of Co nanoparticles into N-doped porous carbon (Co@NPC) nanocages interconnected by carbonized multi-walled carbon nanotubes (C-MWCNTs) are prepared through direct carbonization of the MWCNTs-based ZIF-67 precursor. The obtained hybrid material (denoted as Co@NPC/C-MWCNTs) displays an excellent ORR performance with a half-wave potential of 0.79 V, effective four-electron transfer and superior formate-tolerance ability. The superior ORR activity of the Co@NPC/C-MWCNTs hybrids is mainly ascribed to the abundant catalytic active sites contributed by the Co@NPC nanocages, the high electrical conductivity and large specific surface area rooting in C-MWCNTs, and synergetic effects between Co@NPC nanocages and C-MWCNTs. The membraneless flexible direct formate fuel cell (DFFC) using Co@NPC/C-MWCNTs as the cathode catalyst delivers a peak power density of 4.32 mW cm −2 stably. Notably, the performance of the flexible DFFC can still maintain 90.9% of its initial value after repeated bending for 1000 times. Moreover, two flexible DFFCs connected in series mode can easily power some low-power electronics. The report not only opens a new door to design high-performance non-precious metal ORR catalysts for DFFCs, but also greatly boosts the development of flexible energy conversion and storage devices.

研究领域: 材料科学 · 能源科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Electricity generation property in portable direct formate fuel cells (DFFCs) with polyacrylamide hydrogel

Qiusen Wang,Jianmeng Pang,Yang Yang,Xun Zhu,Dingding Ye,Rong Chen,Qiang Liao

Hydrogel is a type of polymer with three-dimensional network structure, which possesses an internal porous cross-linked structure, good liquid absorption, retention capacity, ion conductivity, and provides stable and rich ion transport paths. Their unique properties guarantee the hydrogels as a transformative platform for next-generation miniaturized electronics. In the study, hydrogel is creatively adopted as the multifunctional electrolyte component instead of membrane, and a novel portable direct formate fuel cell is proposed. The polyacrylamide hydrogels are prepared using a free radical polymerization method, and the liquid retention and ionic conductivity are specifically characterized. A portable fuel cell with the above functional hydrogel is fabricated by integrating the functions of fuel/electrolyte storage, supply and ion-transport. It provides a maximum power density output of 25.31 mW⋅cm −2 and a limiting current density of 145.67 mA⋅cm −2 . The design simplifies the complexity of the fuel cell system, and provides a promising way to power the micro electronic devices.

研究领域: 能源材料科学 · 电化学工程
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

A Na-ion direct formate fuel cell converting solar fuel to electricity and hydrogen

Xianda Sun,Yuxuan Lou,Ya-Ling He,Yinshi Li

The rapid footstep of hydrogen society drives people to pursue the reliable, energy-saving, and renewable hydrogen production patterns. Herein, an electricity-hydrogen co-produced Na-ion direct formate fuel cell (e-h 2 Na-DFFC) is proposed as a conceptual avenue to link the CO 2 utilization and H 2 society. Using the solar fuel-formate that can be readily synthetized from carbon dioxide, we experimentally demonstrate the capability of e-h 2 Na-DFFC for continuous co-production of electricity and hydrogen. A proof-of-concept e-h 2 Na-DFFC yields a peak power density as high as 168 mW cm −2 at 380 mA cm −2 associating with the hydrogen production rate reaching 2.9 mL min −1 cm −2 . More importantly, the approximate 100% purity and over 98.9% Faradic efficiency suggest the great potential of this electricity-hydrogen co-production device. In addition, we explore the scalability, stability and applicability of the e-h 2 Na-DFFC. The hydrogen that is produced from the e-h 2 Na-DFFC can be directly fed to hydrogen-oxygen fuel cell, which presents a peak power density of 546 mW cm −2 and a 35-h stable operation at room temperature . This proposed e-h 2 Na-DFFC provides a new pathway for renewable hydrogen production.

CAS / MDL: 64-17-5 7722-84-1
研究领域: 能源化学 · 可再生能源技术
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2019 · IF 4.084

PdBi alloy nanoparticle-enhanced catalytic activity toward formic acid oxidation

Linyan Hong,Qizhi Dong,Qian Qin,Huizi Li,Jian Xie,Gang Yu,Hong Chen

Improved performance and reduced costs are crucial to develop catalysts for direct formic acid fuel cells. In this study, PdBi alloy nanoparticles were synthesized using a facile seed-mediated growth method. The as-synthesized Pd 1 Bi 1 alloy nanoparticles exhibited a large electrochemical surface area (46.3 m 2  g −1 ) and a high mass activity (1.44 A mg −1 ), which was 1.19- and 4.8-fold higher than that of commercial Pd/C catalysts, respectively. The PdBi alloy nanoparticle is a promising catalyst for direct formic acid fuel cells.

CAS / MDL: 31175-20-9 7440-05-3
研究领域: 材料科学 · 电化学 · 能源科学
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Small Methods · 2023 ·Vol. 7 ·期 7 ·2300021 · IF 12.4

Ultrathin PdCu Nanosheet as Bifunctional Electrocatalysts for Formate Oxidation Reaction and Oxygen Reduction Reaction

Zhipeng Liu,Jinling Xue,Yinshi Li

The development of robust nonplatinum electrocatalysts to enhance the performance of formate oxidation reaction (FOR) and oxygen reduction reaction (ORR) is one of the key issues for the commercialization of direct formate fuel cells (DFFCs), but still challenging. Herein, a structurally controlled 3D flower-like PdCu nanosheet (NS) catalyst is synthesized by a method of oil bath reduction under mild conditions as a bifunctional electrocatalyst for DFFCs. Under the dual tuning on the composition and intermetallic phase, the PdCu nanosheet catalyst exhibits 8.67 times higher mass activity for anodic formate oxidation reaction than the commercial Pd/C. For the cathodic ORR, a positive shift half-wave potential is obtained for PdCu nanosheets exceeding Pt/C. Moreover, after a long-term stability test, the current density of the PdCu nanosheet catalyst for FOR and ORR can be well maintained with the least activity decay. When the PdCu NSs are used as optimized anode and cathode electrodes for DFFCs enable a peak power density as high as 53 mW cm −2 at room temperature, which is about 1.3 times higher than that of the commercial Pd/C and Pt/C as anode and cathode electrodes. This work provides a potential strategy to improve the catalytic performance of non-Pt-based nanocatalysts.

研究领域: 材料科学 · 电化学 · 能源科学
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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 32 ·期 27 ·2201872 · IF 19.924

Novel Superaerophobic Anode with Fern-Shaped Pd Nanoarray for High-Performance Direct Formic Acid Fuel Cell

Yuan Zhou,Yang Yang,Xun Zhu,Tong Zhang,Ding-ding Ye,Rong Chen,Qiang Liao

Direct formic acid fuel cells (DFAFCs) possess the advantages of high power density and theoretical cell potential. Exploring robust catalysts for electrochemical formic acid electro-oxidation (FAO) is greatly essential for the wide spread uptake of DFAFCs. However, many electrodes with attractive catalysts suffer limited mass transport due to sluggish CO 2 bubble growth and departure steps on its surface. In this study, a superaerophobic electrode is developed by depositing fern-shaped palladium nanostructured arrays on the carbon paper (Pd-nanoarray@CP). Its unique superaerophobic feature successfully facilitates the CO 2 bubble releasing from the catalyst surface in a significantly small size. With the merits of specific nanoarray morphology, superior under water superaerophobicity, and rapid gas bubble release, the Pd-nanoarray@CP shows fast charge/mass transport rate, high electrocatalytic activity, and great stability for FAO. A direct formic acid fuel cell equipped with the Pd-nanoarray@CP anode is successfully fabricated on a microfluidic platform. A peak power density of 35.8 mW cm −2 and limiting current density of 173.3 mA cm −2 are obtained, respectively, which are 49.2% and 33.0% higher than that of conventional Pd-black anodes. The electrode with superaerophobic interface allows deeper insight into the mechanism of FAO efficiency and holds promise for possible applications of commercially viable DFAFCs.

CAS / MDL: 64-17-5
研究领域: 材料科学 · 电化学 · 能源技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Designing nanoporous Pd catalyst with dual enhancement of thermodynamics and kinetics for formic acid oxidation reaction

Hualei Wang,Cong Xi,Huiming Yin,Yi Ding

Conventional strategies for developing highly efficient electrocatalysts involve enhancing thermodynamics to minimize overpotential and improving kinetics to maximize reaction current. However, current research on Pd-based catalysts for formic acid oxidation reaction (FAOR) mainly focuses on accelerating its kinetics to increase the peak current. This study proposes a catalyst design that can simultaneously improve the kinetics and thermodynamics of FAOR. Specifically, the home-made catalyst (NPG-Pt 1 -Pd 1 ) is obtained by sequentially depositing monolayer Pt and Pd shells on the surface of nanoporous gold (NPG) substrate. Compared with commercial Pd/C, this electrocatalyst exhibits a noticeable negative shift in onset potential (∼100 mV) and a significantly improved peak current (∼6 times). Experimental data and theoretical calculations demonstrate that NPG-Pt 1 -Pd 1 exhibits a comparatively suitable adsorption energy for small molecules, not only reducing the overpotential but also accelerating the reaction rate of FAOR. Moreover, when applied in direct formic acid fuel cells (DFAFC), the NPG-Pt 1 -Pd 1 anode with an exceptionally low Pd loading of 8.5 μg cm −2 , achieves a remarkable power density of 141 mW cm −2 . The power efficiency of Pd is 230 times that of Pd/C (1 mg cm −2 , 73 mW cm −2 ). Therefore, this work provides a new methodology for developing efficient Pd-based FAOR electrocatalysts .

CAS / MDL: 7601-90-3
研究领域: 材料科学 · 电化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

High performance formic acid fuel cell benefits from Pd–PdO catalyst supported by ordered mesoporous carbon

Yuan Zhou,Xun Zhu,Biao Zhang,Ding-Ding Ye,Rong Chen,Qiang Liao

Formic acid as a renewable fuel can be converted to clean electricity in fuel cells by high-efficient electrochemical oxidation . The conversion rate is fundamentally dictated by the synergy of interactive aspects: catalytic activity , accessibility to active sites, electron transfer , and anti-poisoning stability. For the first time, ordered mesoporous carbon (OMC) is used as the substrate for Pd–PdO catalyst for fuel cells. The unique ordered pore-channel network of OMC can enhance the spatial dispersion of Pd nanoparticles on the pore-channel wall, while the hollow pore-channel can facilitate reactant transport. Microwave and annealing treatments are found to enhance the chemical reduction and to strengthen the anchoring of Pd–PdO catalyst on OMC substrate, respectively. The OMC supported Pd–PdO catalyst (Pd–PdO/OMC) shows 1.7-fold and an order of magnitude higher mass activity and stability as compared to commercial Pd/C catalyst. For fuel cell testing, the Pd–PdO/OMC catalyst is applied to an air-breathing microfluidic fuel cell and achieves a maximum power density of 63.0 mW cm −2 , at least one-fold higher than similar previous reports.

研究领域: 材料科学 · 能源科学 · 电化学
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Journal of the American Chemical Society · 2023 · IF 15

Highly Selective Synthesis of Monoclinic-Phased Platinum–Tellurium Nanotrepang for Direct Formic Acid Oxidation Catalysis

Chengyuan Dong,Xinyao Wang,Zhipeng Zhu,Changhong Zhan,Xin Lin,Lingzheng Bu,Jinyu Ye,Yucheng Wang,Wei Liu,Xiaoqing Huang

Designing efficient formic acid oxidation reaction (FAOR) catalysts with remarkable membrane electrode assembly (MEA) performance in a direct formic acid fuel cell (DFAFC) medium is significant yet challenging. Herein, we report that the monoclinic-phased platinum–tellurium nanotrepang (m-PtTe NT) can be adopted as a highly active, selective, and stable FAOR catalyst with a desirable direct reaction pathway. The m-PtTe NT exhibits the high specific and mass activities of 6.78 mA cm–2 and 3.2 A mgPt–1, respectively, which are 35.7/22.9, 2.8/2.6, and 3.9/2.9 times higher than those of commercial Pt/C, rhombohedral-phased Pt2Te3 NT (r-Pt2Te3 NT), and trigonal-phased PtTe2 NT (t-PtTe2 NT), respectively. Simultaneously, the highest reaction tendency for the direct FAOR pathway and the best tolerance to poisonous CO intermediate can also be realized by m-PtTe NT. More importantly, even in a single-cell medium, the m-PtTe NT can display a much higher MEA power density (171.4 mW cm–2) and stability (53.2% voltage loss after 5660 s) than those of commercial Pt/C, demonstrating the great potential in operating DFAFC device. The in-situ Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy jointly demonstrate that the unique nanostructure of m-PtTe NT can effectively optimize dehydrogenation steps and inhibit the CO intermediate adsorption, as well as promote the oxidation of noxious CO intermediate, thus achieving the great improvement of FAOR activity, poisoning tolerance, and stability. Density functional theory calculations further reveal that the direct pathway is the most favorable on m-PtTe NT than r-Pt2Te3 NT and t-PtTe2 NT. The higher activation energy to produce CO and the relatively weaker binding with CO of m-PtTe NT result in the better CO tolerance. This work achieves remarkable FAOR and MEA performances of advanced Pt-based anodic catalysts for DFAFCs via a phase engineering strategy.

CAS / MDL: 20634-12-2
研究领域: 材料科学 · 电化学 · 催化 · 燃料电池技术
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Materials Today Physics · 2023 · IF 11.5

Hydrogen-intercalation enhanced the anti-CO poisoning ability of palladium-copper metallene for direct formate fuel cells

Hongjie Yu,Shaojian Jiang,Wenjie Zhan,Kai Deng,Ziqiang Wang,You Xu,Hongjing Wang,Liang Wang

The direct formate fuel cells (DFFCs) are energy conversion devices that use formate as fuel. However, CO ads generated from formate dehydration accumulate on the Pd surface and cause catalyst poisoning and deactivation. Here, we constructed a hydrogen intercalated palladium-copper metallene (PdCuH metallene) to enhance the anti-CO poisoning ability. For formate oxidation , the mass and specific activities of PdCuH metallene/C were 3.4 and 3.2 times those of Pd/C. While in ORR , the mass and specific activities of PdCuH metallene reached 12.4 and 13.9 times that of Pt/C. When we assembled PdCuH metallene/C as an electrode material for DFFC, the peak power and limiting current density of PdCuH metallene/C || PdCuH metallene/C were 79.5% and 159.7% higher than that of Pt/C || Pd/C, respectively. This study provides a new resolution to address the CO poisoning deactivation of direct formate fuel cell catalysts.

研究领域: 材料科学 · 能量转换 · 电化学 · 燃料电池
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FUEL · 2025 · IF 7.5

Boron-phosphorus dual-doped graphene supported AuPd nanocatalyst for high-efficiency direct methanol and formic acid fuel cells: Toward sustainable energy solutions

Ze Qin,Henan Shang,Qiuyue Fan,Qi Jia,Lubin Sun,Sijia Li

Direct methanol fuel cells (DMFCs) and direct formic acid fuel cells (DFAFCs) are promising energy conversion technologies due to the high energy density and environmental compatibility. Nevertheless, the widespread application has been hindered by the lack of efficient and durable electrocatalysts capable of simultaneously addressing sluggish reaction kinetics and catalyst poisoning. Herein, a boron-phosphorus dual-doped graphene (BPG) supported AuPd nanoparticles (NPs) is successfully synthesized via a straightforward chemical reduction approach. Au-Pd alloying has modulated the d-band center of Pd, changed the electronic structure of Pd, and also generated a significant bimetallic synergistic effect, thus enhancing the resistance to CO poisoning and improving the performance of the catalyst. Moreover, the BPG support with high defect density and enhanced electron transport capability facilitates uniform nanoparticle dispersion and stabilizes catalytic intermediates. Compared to commercial Pd/C (0.42 A mg Pd -1 for MOR and 0.53 A mg Pd -1 for FAOR), the Au 0.4 Pd 0.6 /BPG catalyst demonstrates superior mass activities of 6.16 A mg Pd -1 for MOR and 10.10 A mg Pd -1 for FAOR . In addition, the Au 0.4 Pd 0.6 /BPG catalyst exhibits excellent long-term durability in both alkaline methanol and acidic formic acid solutions. This study provides a strategic design for supported bimetallic catalysts, which accelerates the development of high-performance fuel cells. This development is consistent with the United Nations Sustainable Development Goals (SDG), specifically SDG 7 (Affordable and Clean Energy) and SDG 13 (Climate Action), by fostering the development of energy conversion technologies that are both low-emission and efficient and that are suitable for off-grid and portable power applications.

CAS / MDL: 10555-76-7
研究领域: 电化学 · 纳米催化 · 能源材料 · 燃料电池 · 表面科学 · 环境友好能源技术
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2016 · IF 3.205

Carbon nanotubes supported platinum–gold alloy nanocrystals composites with ultrahigh activity for the formic acid oxidation reaction

Shu-He Han,Yi-Gang Ji,Shi-Hui Xing,Jiao-Jiao Hui,Qi Guo,Feng Shi,Pei Chen,Yu Chen

Improving the electrocatalytic activity , durability, and utilization of anode eletrocatalysts are crucial for accelerating commercialization of direct formic acid fuel cells. In this work, the multiwall carbon nanotubes (MWCNTs) supported PtAu alloy nanocrystals (MWCNTs/PtAu) composites are synthesized by a one-pot wet-chemical method using polyethyleneimine as the complexant and surfactant . The physicochemical properties of the as-prepared MWCNTs/PtAu composites are characterized detailedly by X-ray diffraction, transmission electron microscopy , scanning electron microscopy, and X-ray photoelectron spectroscopy, etc . These structural investigations display the PtAu alloy nanocrystals are highly dispersed on the surface of the MWCNTs. Cyclic voltammetry and chronoamperometry measurements show the as-prepared MWCNTs/PtAu composites significantly enhance the direct dehydrogenation pathway of the formic acid oxidation reaction, resulting in the improved electocatalytic activity and durability for the formic acid electrooxidation .

CAS / MDL: 9002-98-6
研究领域: 材料科学 · 电化学 · 纳米技术 · 燃料电池
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