CARBON
·
2024
·
IF 10.5
Yongqing Shen,Peizhi Liu,Yangrui Li,Jianghong Wu,Yanhui Song,Junjie Guo
The structural stability of supported metal nanoparticles determines the activity and longevity of heterogeneous catalysts. Unfortunately, the chemical/thermal working environment inevitably accelerates metal sintering to larger crystallites that leads to the degradation of catalytic performance. Here, we demonstrate that the distribution of defects in carbon support as an inherent parameter plays a crucial role in catalyst sintering. Based on in-situ transmission electron microscopy studies, the strong metal-support interaction between platinum (Pt) nanoparticles and defect-rich graphene nanoflakes largely suppresses metal sintering up to 700 °C. Particularly, the optimal carbon support can be achieved in the annealing process, in which the mass transfer and charge transport can be enhanced by accurately manipulating the distribution of defects in carbon matrix and graphitization degree. It is worth noting that the screened Pt/GNs-300 exhibits impressive oxygen reduction reaction performance with high half-wave potential (0.91 V), mass activity (108.1 A g –1 Pt ) and excellent stability. By its ascendancy in ORR, the Pt/GNs-300 exhibits a high open-circuit voltage of 1.41 V and a maximum power density of 198.6 mW cm −2 in Zn-air battery, implying its brilliant practicability. This work paves a pathway for achieving sinter-resistant metal-loaded catalysts in energy electrocatalysis.
研究领域:
材料科学
·
电催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Chao Huang,Yingnan Dou,Liping Sun,Lihua Huo,Qiang Li,Hui Zhao
The mechanism by which the multicomponent systems in high-entropy perovskites regulate catalytic sites remains unclear, especially how the introduction of A-site elements with different radii influences the B-site catalytic centers. This study designed medium-entropy perovskite oxides, (La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 M 0.2 ) 2 NiO 4 (M = Ca, Sr, Ba), by leveraging the differential ionic potentials of strategically selected alkaline earth metals, with the aim of elucidating how systematic modifications of the local polar environment influence the bonding state of catalytic sites and their electrocatalytic behavior. The differing ionic potentials of the A-site cations (Ca, Sr, Ba) modulate the bond strength and electron cloud overlap of the B-site transition metal‑oxygen bonds. This modulation, primarily through coulombic interactions with the B-site metal ions, induces significant electron transfer and consequently adjusts the energy of the d-band center. This weakened interaction facilitates the generation and migration of active oxygen species by lowering the metal‑oxygen bond strength. Electrochemical results indicate that (La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 Ba 0.2 ) 2 NiO 4 (LPNSBNO) exhibits a low polarization resistance of 0.29 Ω cm 2 at 700 °C. The single cell of LPNSBNO achieved a maximum power density of 0.82 W cm −2 in fuel cell mode. A current density of 0.58 A cm −2 was achieved in electrolyzer mode at 1.3 V and 700 °C. Furthermore, compared to Nd 1.6 Ba 0.4 NiO 4 , the entropy-enhanced LPNSBNO exhibits weaker Ba 2+ surface segregation energy, thereby demonstrating more robust Cr/CO 2 resistance. These results establish LPNSBNO as a catalyst with significant potential for bi-functional applications.
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DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 1
·016504
·
IF 4.316
Haomin Jiang,Yujuan Cheng,Zhaohui Wang,Zhiqun Bai,Yang Tang,Yanzhi Sun,Pingyu Wan,Yongmei Chen
The cleavage of the linkage bonds among the C9 units in lignin molecules via selective oxidation method to obtain small-weight aromatic compounds is an important way to lignin valorisation. In this study, the cleavage pathways of bonds in a lignin model compound, GGE (guaiacylglycerol-β-guaiacyl ether), by the reactive oxygen species (ROS) in situ generated through electrochemical oxygen reduction reaction (ORR) in an aprotic ionic liquid ([BMIM]BF4) was investigated. The results indicated that when the main ROS was ·OOH, coniferyl alcohol, guaiacol and vanillin were detected as the degradation products which is supposed to be caused by β-O-4 bonds cleavage; Otherwise, when HO2− was the main ROS, coniferyl alcohol could not be detected and the degradation reaction is believed to be trigerred by Cα-Cβ bonds cleavage.
研究领域:
生物化学
·
环境科学
✓ 已验证
DOI
高影响因子
Functional Materials Letters
·
2023
·
IF 1.3
Huinian Zhang,Suping Jia,Ning Li,Xiaolin Shi,Ziyuan Li
Single-atom catalysts (SACs), especially atomically dispersed Fe–N x –C based SACs, hold great promise to replace Pt-based electrocatalysts for oxygen-reduction reaction (ORR). Currently, synthesizing high-activity ORR electrocatalysts with atomically dispersed Fe–N x site structures is still challenging due to their high surface free energy, which leads to easy migration and serious aggregation. Herein, we have designed a general graphene quantum dots (GQDs)-anchoring strategy to synthesize a single-iron-atom electrocatalyst (Fe–N-GQDs/PC) applied to ORR through calcining of N-GQDs-Fe 3 + modified porous carbon (PC) and melamine. Experiments demonstrate the N-GQDs consist of abundant oxygenated groups, which could lead to complexing metal ions and thus facilitating the formation of SACs. Furthermore, the Fe–N-GQDs/PC electrocatalyst exhibits outstanding electrocatalytic ORR activity in 0.1 M KOH media with half-wave potentials of 0.84 versus 0.85 V for Pt/C. This strategy has opened up new feasible ideas to produce SACs for electrochemical energy devices.
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DOI
高影响因子
Nanoscale Research Letters
·
2019
·Vol. 14
·期 1
·1-11
·
IF 3.159
Guo Chaozhong,Li Yanrong,Xu Ya,Xiang Qin,Sun Lingtao,Zhang Weizhong,Li Wensheng,Si Yujun,Luo Zhongli
Synthesis of metal-free carbon-based electrocatalysts for oxygen reduction reaction (ORR) to replace the conventional platinum-based catalysts has currently become a hot topic of research. This work proposes an activation-assisted carbonization strategy for the fabrication of nitrogen-doped nanoporous carbon microfibers (Me-CFZ-900) with a high BET surface area (~ 929.4 m 2 g −1 ) via using melamine as a promoter/nitrogen source and bamboo-carbon biowastes as the carbon source with the help of a zinc chloride activator. Electrochemical tests showed that the Me-CFZ-900 material has exhibited excellent ORR electrocatalytic activity and long-term stability, and also displayed a quasi-four-electron ORR pathway in alkaline electrolyte. We also find that the graphitic-N may be the catalytically active site for the ORR, but the formation of planar-N can further help to promote the ORR activity for our catalysts. The results open a new space and provide a new idea to prepare valuable porous nanocarbon materials on the basis of carbonaceous solid wastes for catalysis of a wide range of electrochemical reactions in the future.
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 26
·2201263
·
IF 6.389
Mingan Zhou,Minghao Liu,Qiyang Miao,Hengfu Shui,Qing Xu
Oxygen reduction reaction (ORR) plays key roles in fuel cells and metal air batteries. Covalent organic frameworks (COFs)-derived carbons have been utilized for catalyzing ORR. However, the activity and selectivity for these catalysts in the acidic medium is still under improved. In this work, Pt atoms and uniform Pt nanoparticles supported by standing carbons are derived from a three-dimensional COF. With increasing the contents of Pt ions, the corresponding particle sizes show obvious decrease, and thus resulting in higher catalytic activity. The synergetic roles between Pt atoms and nanoparticles with average sizes of 6.19 nm make catalyst show remarkable activity toward ORR, with onset potential and half-wave potential of 0.98 and 0.85 V (vs RHE) in the acidic medium, which are 70 and 40 mV more positive than those of Pt/C, respectively. This work provides a new insight for developing COFs in energy storage and conversion systems.
研究领域:
材料科学
·
能源化学
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Zhiwei Han,Haomin Jiang,Aiguo Xue,Gaoguo Ni,Yanzhi Sun,Yang Tang,Pingyu Wan,Yongmei Chen
Lignin valorization to obtain small aromatic compounds requires selective oxidation to break the linkage bonds among the C9 units in lignin molecules. It has been reported that hydrogen peroxide (H 2 O 2 ) generated through the oxygen reduction reaction (ORR) on the cathode could be an appropriate oxidizing reagent to depolymerize lignin, but the current efficiency was still unsatisfactory. In this study, a protic ionic liquid [Et 3 NH][HSO 4 ] is used as electrolyte instead of aqueous solution, and the generation rate of H 2 O 2 is determined as 0.0563 mmol cm −2 min −1 and the current efficiency of 79.7 % by the Ti-TPyP colorimetric method. Then using p -benzylethoxyphenol (PBP) as a lignin model compound, it is figured out that approximately-two molecules of H 2 O 2 are consumed for breaking one α-O-4 ether bond. Finally, in the electrolysis of an actual lignin sample, it is evaluated that about 19.4 molecules of H 2 O 2 are needed for producing one molecule of vanillin when taking vanillin as a representative degradation product of lignin.
研究领域:
化学工程
·
生物化工
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Huan He,Yongxin Lei,Song Liu,Kunyapat Thummavichai,Yanqiu Zhu,Nannan Wang
The development of low-cost electrocatalysts with high oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) performance is crucial for devices used to convert and store hydrogen energy. Research on OER and ORR catalysts has attracted a lot of attention. The limited single-functional catalysts can be expanded as bi-functional catalysts to meet the extra requirement of preparing high-performance catalysts. In this study, we prepared Co-ZIF/CNF in which carbon nanofibers uniformly encapsulated Co– nanoparticles by electrospinning and simple pyrolysis . Co-ZIF/CNF contains both CoO x and Co-N y active sites, showing bifunctional activity for OER and ORR. The optimized catalyst Co-ZIF 1.5 /10CNF 2 has a low OER overpotential of 390 mV, an onset potential of 0.93 V and a half-wave potential of 0.85 V of ORR, exhibiting an outstanding OER and ORR catalytic performance. The catalyst retained 87.53 % of its current after 12 h, showing great stability. This paper provides a new strategy for designing and preparing OER and ORR bifunctional catalysts.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2023
·Vol. 27
·期 10
·2787-2798
·
IF 2.5
Lei Yimin,Wei Yuxiang,Wu Dekai,Zhu Qing,Sun Yanan,Zhou Xuejiao,Xi He,Zhong Peng,Sun Jie
Electro catalysts play a vital role in facilitating the reaction process in the oxygen reduction reaction (ORR) of fuel cells. In methanol fuel cells, methanol easily penetrates the diaphragm rendering the ORR catalyst inactive. Although commercial platinum exhibits excellent ORR catalytic activity, its poor methanol resistance and long-time durability severely restrict its sustainable development and application. This work synthesized Ti 4 O 7 /CNT nanocomposite electrocatalysts by using the sol-gel method followed by high-temperature carbothermal reduction. The obtained catalysts exhibit a large electrochemically active surface area (347.89 cm 2 ) and low interfacial charge transfer resistance (64.5 Ω). The reduction potential (0.73 V), onset potential (0.93 V), half-wave potential (0.73 V), and electron transfer number (3.7) of this electrocatalyst are all close to those of the Pt/C electrocatalysts in alkaline medium. Simultaneously, it also possesses remarkable methanol tolerance and long-term durability, whose relative current density can maintain above 74% after cycling for 24 h.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 9
·4722-4732
·
IF 5.503
Jizhao Zou,Qi Luo,Hongliang Wu,Shiyu Liu,Tongbin Lan,Yuechao Yao,Muhammad Aurang Zeb Gul Sial,Fenglin Zhao,Qi Zhang,Xierong Zeng
Transition metal selenide-based materials have been demonstrated as promising electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), yet the actual design of a highly efficient and stable electro-catalyst based on these materials still remains a long and arduous challenge. Herein, a predesigned hybrid Zn/Co zeolitic imidazole framework was used to fabricate CoSe2/Co nanoheteroparticles embedded within hierarchically porous Co, N co-doped carbonnanopolyhedra/nanotubes (CoSe2/Co@NC-CNTs) through a facile approach involving controlled carbonization and selenization procedures. As expected, the optimized CoSe2/Co@NC-CNT-1 displayed outstanding electrocatalytic performance for the ORR and OER, with an onset potential of 0.95 V vs. RHE, a half-wave potential of 0.84 V vs. RHE for ORR, and a potential of 1.69 V vs. RHE for OER at 10 mA cm−2. It also exhibited excellent long-term stability and methanol resistance ability, which were superior to commercial IrO2 and the commercial 20 wt% Pt/C catalyst. Notably, the assembled Zn–air battery with CoSe2/Co@NC-CNT-1 showed a low charge–discharge voltage gap (0.696 V at 10 mA cm−2) and a high peak power density (100.28 mW cm−2) with long-term cycling stability. These superior performances can be ascribed to the synergistic effects of the highly active CoSe2/Co nanoheterostructure, hierarchically porous structure with a large surface area, high electrical conductivity and uniform doping of the Co and N.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jifa Dong,Yaming Pang,Denise Bildan,Lu Xing,Xiaoteng Liu,Xiangqun Zhuge,Zhanhui Yuan,Yurong Ren,Dan Liu,Weiwei Lei,Kun Luo
Fe 3 Co nanoparticles have been successfully embedded within ZIF-8 derived carbon nanotube complex using a simple solvent-heated self-assembly-pyrolysis strategy, it acts as an efficient ORR/OER bifunctional electrocatalyst and showed outstanding performance of excellent catalytic activity for ORR (E 1/2 = 0.87 V at 0.1 M KOH) and OER (the overpotential at 10 mA cm −2 is 390 mV at 1 M KOH). Density functional theory (DFT) demonstrates that the introduction of iron and cobalt atoms significantly impacted on the adsorption energies of the reactive intermediates. In particular, the combination of cobalt and iron exhibited significantly enhanced ORR/OER activities, revealing an enhanced effect of synergistic interaction of FeCo site for bifunctional properties. It is used as Fe 3 Co 1 −NC in aqueous zinc-air battery (ZAB) and exhibited a high open-circuit voltage of 1.52 V, power density of 189.8 mW cm −2 , and long cycle durability of 400 h. Flexible ZABs assembled exhibit high power density (81.59 mW cm −2 ) and long cycling durability (90 h).
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Kang Hua,Zhiyan Rui,Tianren Zhang,Yinliang Cao,Xinlong Shen,Shengping Wang,Ping He,Jia Li,Jianguo Liu
Lack of catalytic performance, short life, and high cost are three main problems related to JM-Pt/C catalysts for proton exchange membrane fuel cells. The introduction of cheap transition metals improves catalytic performance while significantly reducing the cost of the catalysts. Here, we report the synthesis of Pt 3 Co/NC alloy catalysts via coating and pyrolysis treatment . The agglomeration of nanoparticles during the high-temperature alloying process is significantly inhibited by coating with PANI . Remarkably, the obtained Pt 3 Co/NC alloy catalysts exhibit excellent ORR catalytic performance and structural stability in 0.1 mol/L HClO 4 . After 30,000 potential cycles, the mass activity and area-specific activity of Pt 3 Co/NC alloy catalysts are 1.949 and 3.936 times higher, respectively, than that of JM-Pt/C with negligible performance loss. The strong metal-support interaction between N and Pt and the Pt-rich surface restrict the dissolution of Pt and Co, resulting in excellent stability. This synthesis approach provides an effective way to develop active and stable Pt alloy catalysts.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）