INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Liping Zhao,Anqi Wang,Ailin Yang,Guihong Zuo,Jun Dai,Youjin Zheng
Exploring electrocatalysts with low cost and excellent performance for oxygen reduction reaction is still a significant challenge. In this paper, we introduce a novel strategy to fabricate ZnS, Fe, and P co-doped N enriched carbon (ZnFeSP/NC) via the direct carbonization of PVP/ZIF-8 combined with absorption, sulphurization , and phosphorization processes. The as-synthesized ZnFeSP/NC was used as electrocatalyst for oxygen reduction reaction (ORR). We explored the influence of Fe, S, and P elements on the ORR activity of the catalysts. It can be found that ZnS nanoparticles were formed and attached on the surface of the ZnFeSP/NC nanoparticles. α-Fe and P element were well dispersed on ZnFeSP/NC nanoparticles. Fe, S, and P element can highly enhance the ORR activity of the catalysts. Compared to Zn/NC, ZnFe/NC, and ZnFeS/CN, ZnFeSP/NC shows the optimal ORR performance with the half-wave potential of 0.859 V and a current density of 3.33 mA cm −2 at −0.85 V. Furthermore, ZnFeSP/NC also exhibits excellent long-term operation stability, effectively avoiding any ORR performance decay.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2019
·
IF 1.901
Xiaoyan Zhang,Xiumei Cheng,Feng Chen,Li Xu,Yaping Wang,Junchao Qian,Zhengying Wu,Qi Zhang
One of the crucial issues in fuel cells is to explore the highly-efficient, long-term stable and low-cost catalysts for the oxygen reduction reaction (ORR). Here, the carbon dots/Co 3 O 4 (CDs/Co 3 O 4 ) is reported as an effective electrocatalyst for ORR. The CDs/Co 3 O 4 was synthesized through an in-situ two-step heating strategy with the graphitic carbon nitride (g-C 3 N 4 ), cobalt nitrate hexahydrate and organic base as raw materials. The carbon dots (CDs) are derived from the C source of g-C 3 N 4 , which are in situ introduced into the Co 3 O 4 to form the CDs/Co 3 O 4 composite. Consequently, the introduction of CDs endows enhanced electrocatalytic activity of the CDs/Co 3 O 4 composite.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2022
·
IF 9.257
Quan Zhou,Yue Yang,Qitong Ye,Tong Xue,Mudong Tu,Yipu Liu,Hua Li,Xiang-Hui Yan,Zhong-Li Zou,Bei-Ping Wang,You-Jun Lu,Feng-Lan Han
Combining catalytic active materials with nitrogen-doped carbon structure has been an effective strategy for designing high-performance electrocatalysts , where N species plays a vital role in modulating the electronic structure of composite material. The N dopant in the carbon structure exists in different states, but it has been ambiguous which type of N structure contributes the most to the overall catalytic activity. Here, Fe 3 C nanoparticles embedded in graphitic nitrogen-dominated carbon framework (Fe 3 C@NC) has been successfully fabricated from Fe@ZIF-8 and exhibits excellent oxygen reduction reaction (ORR) activity and stability. Experiments and theoretical calculations confirm the interaction between Fe 3 C and N-doped carbon. Moreover, graphitic nitrogen is proved to exhibit the highest promotion contribution among different N states, which can effectively reduce the energy barrier of the potential determining step (from O 2 to ∗OOH) for ORR. The Fe 3 C@NC composite is applied as the air cathode in a Zn-air battery, which shows a high E OCV (open-circuit voltage) of 1.48 V, a power density of 155.6 mW/cm 2 , and a specific capacity of 798 mAh/g Zn . This work suggests the synergy of Fe 3 C, N species, and carbon layer in promoting the performance of ORR catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ChemPlusChem
·
2023
·Vol. 88
·期 7
·e202300238
·
IF 3.4
Xingkai Peng,Xiaowei Zhao,Yuekun Hu,Lingli Guo,Yan Liu,Xiaofei Yu,Xiaojing Yang,Xinghua Zhang,Zunming Lu,Lanlan Li
Graphical By adding Zn(OAc) 2 into an amino-enriched reactant system , simultaneous optimization of both porous structure and N-doping process was achieved during the synthesis of porous carbon by the hard template method. The fabricated Zn(OAc) 2 -DCD/HPC catalysts showed excellent ORR activity in alkaline electrolytes. Nitrogen-doped carbon is considered one of the most promising oxygen reduction catalysts due to its low cost and high activity, however, it still falls short of Pt/C. In this study, we report a strategy for the preparation of highly reactive N-doped hierarchical porous carbon by primary pyrolysis using zinc acetate as a stand-alone zinc source and amino-rich reactants as carbon and nitrogen sources to introduce Zn-N x structures into mesoporous structures generated by the hard template method using the strong coordination of zinc and amino groups. Benefited from the simultaneous optimization of the hierarchical porous structure and nitrogen-doping, the half-wave potential of Zn(OAc) 2 –DCD/HPC is as high as 0.909 V vs. RHE, much better than that of commercial Pt/C catalysts (0.872 V vs. RHE). In addition, zinc-air batteries assembled with Zn(OAc) 2 –DCD/HPC (P max =198 mW cm −2 ) as the cathode exhibit higher peak power density compared to Pt/C (P max =168 mW cm −2 ). This strategy might open up new opportunities for designing and developing highly active metal-free catalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NANOTECHNOLOGY
·
2024
·Vol. 35
·期 15
·155401
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IF 2.9
Hongjing Wang,Tongqing Zhou,Shan Xu,Kai Deng,Hongjie Yu,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
The development of effective and stable cathode electrocatalysts is highly desired for fuel cells. Controlling the composition and morphology of Pd-based materials can provide a great opportunity to improve their oxygen reduction reaction (ORR) performance. Here, we report the synthesis of hexagonal close-packed (hcp) Pd2B nanosheet assemblies (Pd2B NAs) via the boronation reaction between as-synthesized Pd NAs and N,N-dimethylformamide. The hcp Pd2B NAs with uniform pore distribution can provide sufficient active sites for ORRs. The insertion of B atoms can induce the phase transition from face-centered cubic structure to hcp structure, as the most thermodynamically stable phase in the Pd-B alloy, which is beneficial for enhancing the ORR stability and toxicity resistance. Therefore, the hcp Pd2B NAs exhibit superior mass activity, specific activity and excellent stability for ORR. The present strategy of boron-intercalation-triggered crystalline transition of Pd-based nanomaterials is valuable for the design of metal–nonmetal catalysts with enhanced performance.
研究领域:
材料科学
·
电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 22
·8803-8811
·
IF 8.262
Tao Fu,Jun Fang,Chunsheng Wang,Jinbao Zhao
Aiming to reduce the dosage of the noble metal Pt and improve the catalytic activity of the catalyst in fuel cells, hollow porous Ag–Pt alloy nanoparticles with Pt coating are prepared via a facile controlled galvanic replacement reaction. Ag is used as the substrate to build a hollow porous structure and alloyed with Pt to minimize the tensile effect of the Ag on the deposited Pt skin which would significantly lower the catalytic performance of the Ag–Pt bimetallic catalyst. This hollow porous Ag/Pt bimetallic catalyst exhibits a long catalytic durability and a mass activity of 0.438 A mgPt−1 at 0.9 V (vs. RHE) towards the oxygen reduction reaction (ORR), which is ca. 3 times higher than that of the commercial Pt/C catalyst. The significant enhancement over the state-of-the-art Pt catalysts can be attributed to (1) the high surface area of the nanoparticles, (2) the more suitable d-band center of the Pt skin deposited on the Ag–Pt alloy substrate, and (3) the high thermal stability of the Ag–Pt alloy. Therefore, this work provides a new strategy for designing high-performance catalysts with low cost. In addition, the synthetic chemistry involved can possibly be extended for fabricating versatile catalysts with a similar structure.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Hua Pan,Xinxing Zhan,Chao Wang,Juan Tian,Zijian Gao,Lingyun Zhou,Yadian Xie,Xin Tong
The interaction between catalysts and supports is recognized as a crucial factor influencing catalytic activity and stability. However, the carbon materials, which have been widely employed as the support at present, encounter challenges including intricate composition and the difficulty of precise control. In this study, the fullerene-derived carbon materials serve as support to electrocatalysts with low platinum. Fullerene-based materials, as the only carbon material with a well-defined molecular structure, have a controllable active site structure, which can provide a reaction model for studying metal-support interactions. Four kinds of fullerene-derived catalysts such as Pt/fullerene, Pt/nitrogen-doped fullerene, Pt/sulfur-doped fullerene, and Pt/phosphorus-doped fullerene, were synthesized. Once the coordination environment of the Pt particles was controlled, thus their catalytic performance was modulated. Despite a platinum loading of only 4.2%, Pt/N-fullerene demonstrates superior oxygen reduction activity and stability compared to commercial Pt/C (20%). Density functional theory calculations show that the introduction of heteroatoms can change the surface charge distribution of fullerenes, in which N-fullerene has a more negative electrostatic potential and can effectively anchor Pt. This research establishes a foundation for understanding the catalysts-support interaction and further precise control of the coordination environment of Pt. This provides new insights for designing efficient ORR catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Xiao Li,Xue-wei Wang,Xiao-Ran Wen,Shi-qi Li,Kun Zhang,Jia-cheng Yu,Yan Guo
Mn-based mullite, with its unique structure featuring two distinct Mn coordination environments, has garnered significant attention in the research and development of oxygen reduction reaction (ORR) catalysts. The nucleation and growth of SmMn 2 O 5 were influenced by controlling the hydrothermal reaction time and temperature, resulting in SmMn 2 O 5 with varying degrees of crystallinity. With the increase of hydrothermal temperature and time, the crystallinity of SmMn 2 O 5 is enhanced, and the morphology changes from an amorphous lamellar structure to a finer and longer nanorod structure. SmMn 2 O 5 with an amorphous lamellar structure prepared at 150 °C for 3 h has a maximum specific surface area of 355.35 m 2 g −1 . The electrochemical results indicate that the amorphous lamellar SmMn 2 O 5 shows excellent ORR performance with a half-wave potential of 0.76 V. This is mainly due to the fact that crystallinity induces an increase in the number of oxygen vacancies, which increases the number of active sites and changes the valence state of Mn. The amorphous lamellar SmMn 2 O 5 was used as a cathode in zinc-air batteries with a power density of 119 mW/cm 2 , showing potential applications. This work demonstrates an effective and simple strategy for increasing the number of oxygen vacancies in SmMn 2 O 5 , which helps the development and application of SmMn 2 O 5 in the field of electrocatalysis.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Guangxu Yao,Jin Wan,Yangjun Luo,Dong Liu,Guolong Qiu,Huijuan Zhang,Yu Wang
Strategic localization of catalytically active sites within single-atom catalyst (SAC) architectures represents a pivotal determinant of material performance, particularly in two-dimensional (2D) substrates like MXenes, which offer intricate structural complexity and multifarious anchoring potentialities. Despite the burgeoning interest in non-metallic single-atom catalysts, a comprehensive understanding of site-specific loading mechanisms and their consequential catalytic implications remains substantially unexplored. Herein, we systematically investigate the precise incorporation of economically viable non-metallic elements—tellurium (Te) and arsenic (As)—onto Ti 3 C 2 MXene, a prototypical 2D material characterized by exceptional structural versatility. Our methodology delineates a nuanced approach to controllable single-atom immobilization, strategically differentiating between vacancy-embedded and surface-supported configurations. Through meticulous experimental design, we demonstrate that Te single atoms strategically integrated within titanium vacancies (C-TeSA-T) manifest superior Oxygen Reduction Reaction (ORR) electrocatalytic performance compared to surface-anchored counterparts (W-TeSA-T). Comprehensive characterization revealed remarkable electrocatalytic metrics, including a half-wave potential of 0.88 V vs. RHE and a limiting current density of 5.65 mA/cm 2 . Synergistic Density Functional Theory (DFT) computations and multi-potential X-ray Photoelectron Spectroscopic (XPS) analyses elucidated the intrinsic mechanistic landscape, conclusively identifying Te single atoms as primary catalytic centers and delineating the rate-determining reaction trajectory. This systematic investigation not only introduces an innovative paradigm for designing cost-effective non-metallic catalysts but also provides fundamental mechanistic insights into the intricate relationship between active site localization and catalytic performance, thereby advancing our fundamental understanding of site-specific catalysis in two-dimensional materials.
研究领域:
材料科学
·
催化化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 30
·2201330
·
IF 6.389
Yaping Wang,Meiyang Liu,Yi Zhang,Qingfeng Yi,Ruowei Yi
Herein, a combined method for planetary ball milling and pyrolysis of g-C 3 N 4 /cobalt phthalocyanine mixture to synthesize Co nanoparticles loaded on C N nanosheets ( g -C 3 N 4 @CoPc- x with different mass ratios x of g-C 3 N 4 :CoPc) is proposed. The synthesized catalysts exhibit a unique 3D open sheet-like structure, and the average size of Co particles is 4.45 nm while encouragingly, a small amount of quasi single-atom cobalt (mean particle size 0.5 nm) is also found in the samples. In addition, the mass ratio of g-C 3 N 4 to CoPc presents a significant effect on ORR activity of the samples. Among the samples, g-C 3 N 4 @CoPc-3 shows excellent ORR performance with the onset potential of 0.94 V in neutral condition and the half-wave potential of 1.00 V in alkaline condition, both better than Pt/C. Its onset potentials in acidic (0.83 V) and alkaline (1.07 V) conditions are also comparable to Pt/C. In a full pH range (acidic, alkaline, and neutral) electrolyte, the prepared samples catalyze ORR via a direct four-electron reaction pathway, and the C 3 N 4 @CoPc-3 reveals high catalytic stability and high anti-alcohol tolerance. Results provide wide feasibility for the synthesis and application of g-C 3 N 4 @CoPc-3 in fuel cells.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nano Research
·
2020
·Vol. 14
·期 4
·1069-1077
·
IF 8.183
Su Panpan,Huang Wenjuan,Zhang Jiangwei,Guharoy Utsab,Du Qinggang,Sun Qiao,Jiang Qike,Cheng Yi,Yang Jie,Zhang Xiaoli,Liu Yongsheng,Jiang San Ping,Liu Jian
Defective electrocatalysts, especially for intrinsic defective carbon, have aroused a wide concern owing to high spin and charge densities. However, the designated nitrogen species favorable for creating defects by the removal of nitrogen, and the influence of defects for the coordination structure of active site and oxygen reduction reaction (ORR) activity have not been elucidated. Herein, we designed and synthesized a pair of electrocatalysts, denoted as Fe-N/C and Fe-ND/C for coordination sites of atomic iron-nitrogen and iron-nitrogen/defect configuration embedded in hollow carbon spheres, respectively, through direct pyrolysis of their corresponding hollow carbon spheres adsorbed with Fe(acac) 3 . The nitrogen defects were fabricated via the evaporation of pyrrolic-N on nitrogen doped hollow carbon spheres. Results of comparative experiments between Fe-N/C and Fe-ND/C reveal that Fe-ND/C shows superior ORR activity with an onset potential of 30 mV higher than that of Fe-N/C. Fe-ND sites are more favorable for the enhancement of ORR activity. Density functional theory (DFT) calculation demonstrates that Fe-ND/C with proposed coordination structure of FeN 4− x (0< x <4) anchored by OH as axial ligand during ORR, weakens the strong binding of OH* intermediate and promotes the desorption of OH* as rate-determining step for ORR in alkaline electrolyte. Thus, Fe-ND/C electrocatalysts present much better ORR activity compared with that of Fe-N/C with proposed coordination structure of FeN 4 .
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
·
2013
·
IF 5.008
Jiaoxing Xu,Yi Zhao,Cai Shen,Lunhui Guan
Development of inexpensive and sustainable cathode catalysts that can efficiently catalyze the oxygen reduction reaction (ORR) is of significance in practical application of fuel cells. Herein we report the synthesis of sulfur and nitrogen dual-doped, ordered mesoporous carbon (SN-OMCs), which shows outstanding ORR electrocatalytic properties. The material was synthesized from a surface-templating process of ferrocene within the channel walls of SBA-15 mesoporous silica by carbonization, followed by in situ heteroatomic doping with sulfur- and nitrogen-containing vapors. After etching away the metal and silica template, the resulting material features distinctive bimodal mesoporous carbon frameworks with high nitrogen Brunauer–Emmett–Teller specific surface area (of up to ∼1100 m2/g) and uniform distribution of sulfur and nitrogen dopants. When employed as a noble-metal-free electrocatalyst for the ORR, such SN-OMC shows a remarkable electrocatalytic activity; improved durability and better resistance toward methanol crossover in oxygen reduction can be observed. More importantly, it performs a low onset voltage and an efficient nearly complete four-electron ORR process very similar to the observations in commercial 20 wt % Pt/C catalyst. In addition, we also found that the textural mesostructure of the catalyst has superseded the chemically bonded dopants to be the key factor in controlling the ORR performance.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）