MOLECULES
·
2023
·Vol. 28
·期 7
·2879
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IF 4.6
Sensen Li,Yan Lv,Sawida Elam,Xiuli Zhang,Zhuojun Yang,Xueyan Wu,Jixi Guo
The rational design of morphology and structure for oxygen reduction reaction (ORR) catalysts still remains a critical challenge. Herein, we successfully construct defect-rich and hierarchically porous Fe-N-C nanosheets (Fe-N-CNSs), by taking advantage of metal-organic complexation and a mesoporous template. Benefiting from the advantages of high density of active sites, fast mass transfer channels, and sufficient reaction area, the optimal Fe-N-CNSs demonstrate satisfactory ORR activity with an excellent half-wave potential of up to 0.87 V, desirable durability, and robust methanol tolerance. Noteworthy, the Fe-N-CNSs based zinc–air battery shows significant performance with a peak power density of 128.20 mW cm−2and open circuit voltage of 1.53 V, which reveals that the Fe-N-CNSs catalysts present promising practical application prospects. Therefore, we believe that this research will provide guidance for the optimization of Fe-N-C materials.Keywords:electrocatalytic;Fe-N-C materials;oxygen reduction reaction;two-dimensional materials
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
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 39
·20922-20931
·
IF 8.867
Jieyu Liu,Meng Yu,Xuewei Wang,Jie Wu,Changhong Wang,Lijun Zheng,Dachi Yang,Hui Liu,Yan Yao,Feng Lu,Weichao Wang
An alternative material SmMn2O5 mullite with regard to Pt/C is proposed to catalyze the oxygen reduction reaction (ORR) by combining density functional theory (DFT) calculations and experimental validations. Theoretical calculations are performed to investigate the bulk phase diagram, as well as the stability and electrocatalytic activity of the ORR under alkaline conditions for SmMn2O5 (001) surfaces, which are passivated by nitrogen atoms to avoid any spurious interference. The adsorptions of relevant ORR species (O*, OH*, OOH* and OO*) tend to compensate the coordination of manganese atoms to form Mn-centered octahedral or pyramidal crystal fields, and the corresponding binding energies fulfill a linear relationship. An oxygen molecule prefers to be reduced to OH−via a four-electron pathway and this prediction is verified by electrochemical measurements on the as-prepared SmMn2O5 catalyst with a nanorod structure. Volcano curves are obtained to describe the trends in theoretical ORR activity as a function of a single parameter, i.e. the oxygen binding energy. An overpotential of 0.43 V is obtained at the O* binding energy around 3.4 eV, which is close to the experimental observation (0.413 V) in this work. SmMn2O5 mullite exhibits favorable ORR activity and superior stability with only ∼5% decay in activity over 20 000 s of chronoamperometric operation in contrast to ∼15% decrease of Pt/C, making it a promising candidate for a cathode catalyst.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2014
·
IF 5.9
Pengfei Zhang,Yutong Gong,Zhongzhe Wei,Jing Wang,Zhiyong Zhang,Haoran Li,Sheng Dai,Yong Wang
The development of meaningful ways to transfer biomass into useful materials, more efficient energy carriers, and/or carbon storage deposits is a profound challenge of our days. Herein, an ionothermal carbonization (ITC) method, via treating natural resources (glucose, cellulose, and sugar cane bagesse) in nonmetal ionic liquids (ILs) at ∼200 °C, is established for the fabrication of porous heteroatom-doped carbon materials with high yield. Commercial ILs with bulky bis(trifluoromethylsulfonyl)imide anion or cross-linkable nitrile group were found to be efficient and recyclable templates for porosity control, leading to exciting nanoarchitectures with promising performance in oxygen reduction reaction. The optimized ILs (12 mL) can dissolve and directly convert up to 15 g of glucose into porous carbon materials (SBET: 272 m2/g) one time. This ITC method relies on the synergistic use of structure-directing effect, good biomass solubility, and excellent thermal stability of ILs, and provides a sustainable strategy for exploiting biomass.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 41
·21709-21714
·
IF 8.867
Ergui Luo,Meiling Xiao,Junjie Ge,Changpeng Liu,Wei Xing
Developing cost-effective and highly efficient oxygen reduction electrocatalysts, such as non-precious metal and metal-free catalysts, is undoubtedly crucial for the commercialization of low-temperature fuel cells. Here, edge-rich nitrogen doped porous carbon catalysts for the oxygen reduction reaction (ORR) with a high proportion of pyridinic and pyrrolic N (up to 94%) were synthesized by an in situ released CO2 activation method, using glucose and melamine as precursors and nano-CaCO3 as the template. The catalysts exhibit a three-dimensional structure, hierarchical pores and large pore volumes. Benefiting from the increased active site density and structural advantage, the optimized catalyst shows excellent ORR activity with a half-wave potential of 0.853 V and long-term stability in alkaline media, which is among the best for metal-free catalysts reported to date.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Ruihui Gan,Yali Wang,Wenjun Ma,Mahmut Dirican,Sa Zhao,Yan Song,Xiangwu Zhang,Chang Ma,Jingli Shi
It is highly desirable to develop high-efficiency non-precious electrocatalysts toward oxygen reduction reaction (ORR). In this work, Fe 2 O 3 -encapsulated and Fe-Nx-containing porous carbon spheres (Fe 2 O 3 /N-MCCS) with unique multi-cage structures and high specific surface area (1360 m 2 g −1 ) are fabricated. The unique porous structure of Fe 2 O 3 /N-MCCS ensures fast transportation of oxygen during ORR. The combined effect of Fe 2 O 3 nanoparticles and Fe-Nx configurations endows Fe 2 O 3 /N-MCCS (E 1/2 = 0.837 V vs. RHE) with superior ORR activity and methanol tolerance to Pt/C. And, Fe 2 O 3 /N-MCCS exhibits better stability than nitrogen-modified carbon. The characterization results of Fe 2 O 3 /N-MCCS after long-term test reveals its excellent structural stability. Impressively, zinc-air battery based on Fe 2 O 3 /N-MCCS showed a peak power density of 132.4 mW cm −2 and a specific capacity of 797 mAh g −1 , respectively.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 5
·2101831
·
IF 6.389
Dekai Wu,Chengzhe Yang,Jie Sun,Peng Zhong,Xiaohua Ma,Yimin Lei
In this paper, Ti 4 O 7 /g-C 3 N 4 nanocomposites are successfully prepared by hydrothermal and carbothermal reduction reaction. It shows large specific surface area and electrochemical active surface area (ECSA = 187.82 cm 2 ) and can act as an oxidation reduction reaction catalyst. Compared with commercial Pt/C catalyst, Ti 4 O 7 /g-C 3 N 4 nanocomposites show good catalytic activity in alkaline medium. The peak potential, onset potential, and half-wave potential are 0.74 (versus RHE), 0.96 (versus RHE), and 0.74 V (versus RHE), respectively. It is worth mentioning that Ti 4 O 7 /g-C 3 N 4 catalyst shows better methanol tolerance and cycle stability than commercial Pt/C catalyst. The relative current density attenuation is less than 30% after a long cycle of 24 h.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2022
·
IF 4.383
Shaohui Zhang,Hao Cui,Haikun Zhou,Xiyu Tan,Pengfei Tan,Jun Pan
Platinum-based alloy nanowires are often employed in oxygen reduction reaction (ORR) due to their exceptional performances. However, most platinum-based alloy nanowires suffer from poor stability in strong acidic electrolytes, as well as their complex preparation methods. Herein, PtMn@Pt core-shell nanowires were successfully prepared by one-step hydrothermal with different concentrations of polyvinylpyrrolidone (PVP) and replacement reaction. The results show that the microstructure of nanowires gradually change with the increase of PVP concentration. Meanwhile, the outer layer of the PtMn nanowires contains a Pt-skin of about 1–2 nm. Moreover, the mass activity of the prepared PtMn@Pt core-shell nanowires with 50 mg PVP is 0.409 A mg −1 (@0.9 V), which is 3.86 times higher than that of commercial Pt/C. The as-prepared nanowires display excellent stability mainly due to the existence of Pt-skin. This paper provides a relatively simple method to synthesize Platinum-based core-shell nanowires with outstanding ORR performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Tengda Lu,Lele Yang,Xiao Chen,Mian Li,Lina Han,Chengxu Zhang,Peng Dong,Jie Xiao,Xiaoyuan Zeng,Yingjie Zhang
The negative effects of the widespread and rough use of fossil energy have promoted the emergence of new energy technologies. Cost-effective electrocatalysts play an irreplaceable role in energy conversion and storage , especially oxygen reduction reactions (ORR) catalysts. While the reserves of precious metal catalysts are rare and expensive, it is of prime importance to develop catalysts that can replace precious metals. In the present work, La 0.8 Sr 0.2 Mn 0.8 Co 0.2 O 3-δ (LSMC) with Mn and Co is successfully prepared by sol-gel method and subsequent calcination . The characterizations of physical phase, microstructure, BET and valence state of elements demonstrate that LSMC material possesses ample mesoporous structure, large specific surface area, and multivalent elements, which can provide abundant active sites for ORR. The electrochemical tests reveal that the LSMC delivers outstandingly higher electrocatalytic activity for ORR, relatively lower overpotential and Tafel slope and a better long-term stability than the other perovskites (LSM, LSC) under alkaline condition. Furthermore, the coupling effects of high content of high-valence Co, multivalent Mn and large amounts of adsorbed oxygen endow the catalyst excellent ORR electrocatalytic activity. The present work investigating the effect of Mn and Co elements on the electrocatalysis of LSMC perovskite, will provide the possibility of developing a new type of perovskite electrocatalyst with excellent ORR electrocatalytic activity and low cost.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Siyu Chu,Min Sun,Zijiong Li,Haiyan Wang,Feng Miao
The carbon-based catalysts exhibit excellent electrocatalytic and stable performance toward oxygen reduction reaction (ORR), which are expected to replace expensive and scarce Pt-based catalysts. However, how to regulate the interaction between silver and carrier carbon dots (CD) to improve electrocatalytic performance toward oxygen reduction reaction (ORR) and stability, has not been systematically studied. In this study, we in-situ synthesized fluorine and nitrogen co-doped CD anchoring Ag nanoparticles by UV irradiation reduction method. The peak potential, onset-potential and half-wave potential of F, [email protected] are 0.85 V, 1.056 V, and 0.9 V, respectively, indicating outstanding ORR performance. The current density of F, [email protected] remains 97.5 % after 50, 000 s, showing more excellent stability than Pt/C. The impressive ORR catalytic activity and stability of F, [email protected] could be attributed to the strong anchoring effect of nitrogen-doped CD on Ag. This effect leads to a significant interaction and charge transfer between Ag and CD, thereby enhancing the charge transfer process during the catalytic reaction. This project aims to design a carbon dot/silver composite catalyst with high ORR catalytic performance and favorable stability. The implementation of this project provides good theoretical guidance for the design of carbon nanomaterial-based catalytic systems.
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
·
2024
·
IF 8.3
Yajie Guo,Fuxian Zheng,Ting Wang,Xinyang Liu,Xiaotan Tian,Konggang Qu,Lei Wang,Rui Li,Wenjun Kang,Zongge Li,Haibo Li
Palladium (Pd)-transition metal alloys have the potential to regulate the intermediate surface adsorption strength in oxygen reduction reactions (ORR), making them a promising substitute for platinum-based catalysts. Nonetheless, prolonged electrochemical cycling can lead to the depletion of transition metals, resulting in structural degradation and poor durability. Herein, the synthesis of alloy catalysts (Pd25%Te75%) containing Pd and the metalloid tellurium (Te) through a one-step reduction method is reported. Characterizations of powder X-ray photoelectron spectroscopy, X-ray diffraction, and high-resolution transmission electron microscopy demonstrated both uniform dispersion and strong binding force of elements within the PdTe alloy, along with providing crystallographic details of associated compounds. Based on density functional theory calculations, PdTe had a more negative d-band center than that of pure Pd, which reduces the adsorption capacity between active sites and intermediates in the ORR, and therefore enhances reaction kinetics. The Pd25%Te75% exhibited excellent ORR activity, and its onset and half-wave potentials were ∼0.98 and ∼0.90 V, respectively, at 1600 rpm within the O2-saturated 1.0 M KOH. Significantly, accelerated durability tests achieved exceptional stability, and half-wave potential just decayed by 4 mV after 30000 consecutive cycles. Moreover, this study aims to promote the preparation of Pd and metalloid alloys for other energy conversion applications.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Congyue Sun,Zhongcheng Zhao,Dongyan Xu,Xiaojin Li,Ke Ye
The rapid development of proton-exchange membrane fuel cells needs to develop Pt-based oxygen reduction reaction (ORR) catalysts with activity and stability. In this study, PtCu alloy nanoparticles were in situ anchored on an N-doped porous carbon (NC) derived from ZIF-8 with a chemical reduction method to produce a PtCu/NC catalyst with a Pt loading of 7.96 wt %. The PtCu alloy nanoparticles are uniformly immobilized on the NC with a high surface area via a metal–support interaction. The electrochemical test results demonstrated that the PtCu/NC catalyst displays remarkable activity with an E1/2 value of 0.913 V vs RHE, higher than 0.878 V vs RHE for the commercial Pt/C. The ORR mass activity of the PtCu/NC catalyst is 1.49 and 6.54 times that of PtCu/XC-72 and commercial Pt/C, respectively. The eminent ORR performance of PtCu/NC is attributed to the high specific area of NC and electron-rich Pt sites enhanced by electron transfer from the N and Cu atoms. Moreover, PtCu/NC exhibited better catalytic stability than PtCu/XC-72 and Pt/C after 3000 potential cycles, attributed to the interaction between the N atom and PtCu alloy.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Yunfeng Zhan,Xiang Yu,Linmin Cao,Bodong Zhang,Xiaoxian Wu,Fangyan Xie,Weihong Zhang,Jian Chen,Weiguang Xie,Wenjie Mai,Hui Meng
The nitrogen doping effect on a kind of graphitic carbon as non noble metal catalyst for the oxygen reduction reaction is studied. Glycine and NH 3 are chosen as different nitrogen source and different doping sequences are applied. The structural defect of graphitic carbon, total nitrogen content, types of nitrogen species and surface area are different from different treatment. Glycine will not influence the structure of graphitic carbon but NH 3 introduces defects. Glycine introduces high content of nitrogen to graphitic carbon but NH 3 introduces no nitrogen. The best catalyst is prepared by doping graphitic carbon with glycine first then heat treated with NH 3 . Some of the nitrogen species can be removed by further NH 3 treatment, but the relative content of graphitic nitrogen increases, together with increased surface area result in higher activity.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
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