Journal of Energy Chemistry
·
2020
·
IF 7.216
Xiaojing Jiang,Jianian Chen,Fenglei Lyu,Chen Cheng,Qixuan Zhong,Xuchun Wang,Ayaz Mahsud,Liang Zhang,Qiao Zhang
Controllable fabrication of Fe-N-C based single-atom catalysts (SACs) for enhanced electrocatalytic performance is highly desirable but still challenging. Here, an in situ surface-confined strategy was demonstrated for the synthesis of single atomic Fe-N 4 on N-doped carbon nanoleaves (L-FeNC). The in situ generated Zn 3 [Fe(CN) 6 ] 2 could not only serve as a protection layer against collapse of nanoleaves but also provide abundant Fe source for the formation of Fe-N moieties during pyrolysis, leading to high surface area and high graphitization degree of L-FeNC simultaneously. Benefiting from abundant Fe-N 4 active sites, enhanced mass and charge transfer, the as-prepared L-FeNC manifested a half-wave potential of 0.89 V for oxygen reduction reaction (ORR) in 0.1 M KOH. A maximum power density of 140 mW cm −2 and stable discharge voltage even after operation for 50,000 s have been demonstrated when the L-FeNC was used as air cathode for Zn-air battery. This work not only provided a unique surface-confined strategy for the synthesis of two-dimensional nanocarbons, but also demonstrated the significant benefit from rational design and engineering of Fe-N-C SACs, thus offering great opportunities for fabrication of efficient energy conversion and storage devices.
研究领域:
材料科学
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电化学
·
能源存储与转换
·
纳米科技
·
催化化学
✓ 已验证
DOI
高影响因子
TETRAHEDRON
·
2014
·Vol. 70
·期 47
·9033-9040
·
IF 2.817
Tao Liu,Meng-Meng Liu,Xiao-Wen Zheng,Chong-Yang Du,Xiang-Yang Cui,Lu Wang,Ling-Li Han,Zhang-Yu Yu
The redox reactions of p -hydroquinone and pyrocatechol undergo a two-proton-two-electron process in aqueous solution. We calculated their redox potentials at the B3LYP/6-311+G(d,p) level, and verified the values by employing cyclic voltammetry experiments. Then we selected seven substituent groups (–F, –Cl, –OH, –COOH, –CN, –NH 2 , and –NO 2 groups) to systematically investigate the substituent effect , including the sort, position, and number of the substituent, on the redox potentials of p -hydroquinone and pyrocatechol. The calculated results show that –NH 2 and –OH groups can decrease the redox potentials, while –F, –Cl, –COOH, –CN, and –NO 2 groups increase the potential values of p -hydroquinone and pyrocatechol. The calculations can accurately predict the substituent effects on the redox potentials of pyrocatechol and p -hydroquinone. We would expect that the accurate calculation results for the model systems could be applied in the prediction of electrode potentials of other molecules.
研究领域:
物理有机化学
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电化学
·
计算化学
·
分子设计
·
生物电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Hongguan Li,Jing Wang,Ruijuan Qi,Yongfeng Hu,Jing Zhang,Hongbin Zhao,Jiujun Zhang,Yufeng Zhao
Charge and spin manipulations of electrons are considered to be of great significance in boosting the catalytic activity of M N C electrocatalysts. However, to the best of our knowledge, most current studies focus only on the charge engineering, the interplay between spin and charge is not well understood, and the simultaneous manipulation of both charge and spin remains challenging. Herein, we show that the cooperative interplay between charge itineration and spin-polarization of electrons has a profound impact on the catalytic behavior through density functional theory (DFT) calculations for the first time. Following this concept, we report a Fe-Ni atomic pair as a superior bifunctional catalyst for high performance ORR and OER, with a very small potential difference (ΔE) of 0.691 V. We confirm that the coexistence of Fe 3d itinerant charge and moderate spin polarization (magnetic moment: 1.48 μ B ) is responsible for the superior functional catalytic activity for the Fe Ni atomic pairs.
研究领域:
电催化
·
材料化学
·
物理化学
·
纳米催化
·
能源材料
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计算化学
✓ 已验证
DOI
高影响因子
Science China-Materials
·
2021
·Vol. 65
·期 3
·721-731
·
IF 8.273
Xu Hui,Jin Meng,Geng Jing,Zhang Shengbo,Zhang Haimin
The decentralized production of H 2 O 2 via a two-electron oxygen reduction reaction (2e − ORR) has emerged as a promising alternative to the energy-intensive anthraquinone (AQ) process. However, its practical application requires 2e − ORR electrocatalysts with high activity and selectivity. Herein, we report the synthesis of metallic Ni nanoparticles anchored on bacterial cellulose-derived carbon fibers (Ni-NPs/BCCF) via a facile impregnation-pyrolysis method as efficient electrocatalysts for 2e − ORR to H 2 O 2 . By tuning the amount of Ni precursor, the best electrocatalytic performance toward 2e − ORR was achieved for Ni-NPs/BCCF-20.7, affording a high H 2 O 2 selectivity of ∼90% and an onset potential of 0.75 V vs. reversible hydrogen electrode (RHE) in an alkaline electrolyte. Ni-NPs/BCCF-20.7 achieved the largest H 2 O 2 yield rate of 162.7 ± 13.7 mmol g cat −1 h −1 and the highest Faradaic efficiency of 93.9% ± 4.2% at 0.2 and 0.5 V vs. RHE from the bulk ORR system, respectively. Theoretical calculations revealed the more favorable “end-on” adsorption configuration of molecular oxygen on the exposed Ni(111) plane, which can effectively suppress the O-O bond dissociation, resulting in high selectivity for H 2 O 2 generation.
研究领域:
材料化学
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电化学
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纳米催化
·
能源科学
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环境工程
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2021
·Vol. 47
·期 15
·21459-21465
·
IF 4.527
Xianwei Su,Xiaojia Shang,Yusi Che,Shaolong Li,Jianxun Song,Jilin He
Homogenous ZrC x O y powders have been successfully synthesized by in-situ electro-reduction of solid ZrO 2 –C composite precursors in molten CaCl 2 . The effect of applied cell voltage and molar ratio of ZrO 2 to C on preparation of ZrC x O y were investigated. The reduction pathway of the composite electrode was studied based on the analysis of intermediate products using X-ray diffraction (XRD) and scanning electron microscopy (SEM). The results show that ZrO 2 is firstly converted to CaZrO 3 . The resulting CaZrO 3 is then reduced to ZrC x O y . The ZrC x O y formation is dramatically influenced by electrolysis voltage and molar ratio of ZrO 2 to C: a higher cell voltage and lower molar ratio of the ZrO 2 to C are more preferable for the formation of ZrC x O y powder. Homogenous ZrC x O y powders with particle size of ~100 nm are synthesized by ZrO 2 /C starting elemental powders in CaCl 2 molten salt at 1123 K for more than 3 h, when the cell voltage is 3.0 V and the molar ratio of the ZrO 2 to carbon starting materials is 1:1.0.
研究领域:
材料科学
·
无机非金属材料
·
电化学合成
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粉末冶金
·
固态化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Hui Wang,Houzhen Chen,Hongjiao Wang,Lei Wu,Qixing Wu,Zhongkuan Luo,Fang Wang
The electrochemical performance of the lithium−oxygen (Li−O 2 ) batteries largely depends on the material and architecture of the catalytic cathode. In this paper, to avoid the parasitic reactions of carbon and binder with discharge products and reaction intermediates, we proposed an effective design of a free-standing catalytic cathode for Li−O 2 batteries. The FeCo 2 O 4 @Ni electrode consists of FeCo 2 O 4 nanosheets grown directly on nickel (Ni) foam. The resultant hierarchical macroporous/mesoporous structure provides sufficient space for the insoluble discharge product Li 2 O 2 and catalytically active sites for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Consequently, the carbon- and binder-free self-supporting electrode has demonstrated a high discharge capacity with relatively low charge overvoltage and a better cycle performance than the corresponding carbon-based electrodes.
研究领域:
电化学
·
能源材料
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纳米材料
·
电催化
·
储能技术
✓ 已验证
DOI
高影响因子
ADVANCED POWDER TECHNOLOGY
·
2019
·Vol. 30
·期 9
·1920-1931
·
IF 3.25
Ting Wang,Bing–rui Li,Li–guang Wu,Yu–bing Yin,Bo–qiong Jiang,Ju–qing Lou
La 3+ - or Yb 3+ -doped TiO 2 supported on the surface of reduced graphene oxide were fabricated by adsorbed-layer nanoreactor synthesis (ANS) coupling with a solvothermal treatment to extend photocatalysis application in the advanced treatment of simulated wastewater with high salt concentration. Results showed that La 3+ or Yb 3+ could distribute in the TiO 2 lattice, only in ANS preparation with graphene oxide as the carrier, to replace Ti 4+ during the solvothermal treatment, thus introducing TiO 2 mixed-crystal and heterojunction structures in the catalysts. La 3+ or Yb 3+ caused lattice distortion structures and anionic vacancies in the TiO 2 lattice. The anionic vacancies (oxygen vacancies) might generate Ti 3+ in catalysts, thus enhancing visible-light response, due to impurity levels introduced by La 3+ or Yb 3+ . As the strong adsorption capability of the catalyst for phenol was not interfered by salt ions in the simulated wastewater, the catalysts could efficiently degrade phenol. The highest removal rate of phenol was approximately 90%.
研究领域:
环境科学
·
材料化学
·
光催化
·
水处理
·
纳米材料
·
表面化学
·
环境功能材料
✓ 已验证
DOI
高影响因子
ORGANIC ELECTRONICS
·
2019
·
IF 3.495
Xiangli Gao,Gaoyi Han,Yunzhen Chang,Ying Zhang,Honggang Li
To enhance the reduced graphene oxide hydrogels' capacitive performance, many modifiers are used to add doped element into the materials and improve the structure. The isomers of aminophenol which contain amino and hydroxyl groups on the benzene ring are employed as structure regulator and modifier to synthesize high-performance reduced graphene oxide hydrogels. The influences of preparation conditions including ratios of graphene oxide to aminophenol isomers, temperature, reaction times on the samples’ structure and properties have been investigated. The results show that the oligomer of o-aminophenol is formed on reduced graphene oxide sheets while the molecules of p, m-aminophenol are bound to the sheets; and that the hydrogel prepared in the presence of p-aminophenol has larger specific surface area, total pore volume , specific capacitance and good rate capability (74.0% of 427.0 F g −1 retains at 100 mV s −1 ) than other. The cells assembled by the optimized hydrogels exhibit the energy density of 14.07 Wh kg −1 at power density of 124.3 W kg −1 , and 4.96 Wh kg −1 at 6.78 kW kg −1 . Furthermore, 92.2% of initial capacitance can be retained after 20,000 cycles for the cells assembled by the optimal hydrogel. This kind of material may be found its use in energy storage field.
研究领域:
材料科学
·
纳米科技
·
电化学
·
能源存储
·
高分子化学
·
表面科学
✓ 已验证
DOI
高影响因子
Nano Energy
·
2020
·
IF 16.602
Qingyan Zhou,Zhen Zhang,Jiajun Cai,Bing Liu,Yunlong Zhang,Xiaofei Gong,Xulei Sui,Aiping Yu,Lei Zhao,Zhenbo Wang,Zhongwei Chen
Rational design and construction of highly efficient and durable non-noble-metal bifunctional catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial to promote the widespread implementation of rechargeable Zn-air batteries. Herein, a bifunctional catalyst comprising Co nanoparticles uniformly embedded in hollow nitrogen doped carbon tubes (Co@hNCTs) is fabricated by a facile tube-directed templating strategy. In this strategy, surfactant-treated polypyrrole (PPy) nanotubes serve as the structure-guiding templates for efficient capture of Co 2+ , realizing the in-situ growth of zeolitic imidazolate frameworks-67 (ZIF-67) nanocrystals on PPy nanotubes . Sodium laurylsulfonate acts as anionic surfactant to endow PPy nanotubes with functional electronegative surface and strong anchoring effect toward ZIF-67, playing the pivotal role in binding of ZIF-67 nanocrystals with PPy nanotubes potently. Consequently, the developed catalyst presents a superior ORR activity with the half-wave potential of 0.87 V excellent durability with only a 7 mV loss of half-wave potential after 5000 cycles. The catalyst also exhibits superior catalytic performance for OER. When serving as an air electrode in Zn-air batteries, a large power density of 149 mW cm −2 and long-term cyclability for over 500 h are realized in ambient air, implying the great potential in practical application.
研究领域:
材料科学
·
电化学
·
能源存储
·
催化化学
·
纳米材料
✓ 已验证
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 118
·97256-97263
·
IF 3.84
Qianqian Huang,Weiqiang Yu,Rui Lu,Fang Lu,Jin Gao,Hong Miao,Jie Xu
Catalytic conversion and application of bio-based platform chemicals is of great significance. Itaconic acid, one of the abundant and renewable bio-based platform chemicals, could be hydrogenated to produce methylsuccinic acid, which has important applications in pharmaceutical synthesis. Traditional catalysts can be corroded, leached and deactivated in an acid reaction environment, and the stability of the catalysts is a great challenge. Carbothermal reduction was employed to prepare stable ruthenium-based catalysts, and the results confirmed that CO generated in situ functioned as an efficient reducing species in the carbothermal reduction process. The catalysts were applied for the hydrogenation of itaconic acid, and showed good stability and resistance to acid with no obvious loss of activity and less leaching in recycling tests compared to hydrogen reduced samples which exhibited an apparent decrease of 22% for the conversion of itaconic acid. The carbothermal reduced catalysts could maintain 99% conversion and 99% selectivity for methylsuccinic acid, and maintained good stability and acid-resistance under a higher temperature and longer reaction time.
研究领域:
催化化学
·
绿色化学
·
生物质转化
·
有机合成
·
材料化学
·
工业催化
·
可持续能源
✓ 已验证
DOI
高影响因子
MATERIALS LETTERS
·
2016
·
IF 2.437
Bin Xu,Tao Ding,Yongcai Zhang,Yaoting Wen,Zhanjun Yang,Ming Zhang
This communication reports the development of a new efficient visible-light-driven composite photocatalyst comprising ZnFe 2 O 4 nanoparticles and conjugated polymer (CPVC) from the dehydrochlorination of polyvinyl chloride (PVC). ZnFe 2 O 4 /CPVC nanocomposites were synthesized via three main steps: (i) the synthesis of ZnFe 2 O 4 nanoparticles by a sol-gel method; (ii) the adsorption of PVC in tetrahydrofuran solution by ZnFe 2 O 4 nanoparticles to form ZnFe 2 O 4 /PVC nanocomposites; and (iii) the dehydrochlorination of PVC in the ZnFe 2 O 4 /PVC nanocomposites by heating at 150 °C for 2 h. X-ray diffraction, Fourier transform infrared spectroscopy and high-resolution transmission electron microscopy characterization revealed that the as-synthesized product was core/shell structured ZnFe 2 O 4 /CPVC nanocomposites. The photocatalytic results demonstrated that the ZnFe 2 O 4 /CPVC nanocomposites had much higher photocatalytic activity than ZnFe 2 O 4 nanoparticles in the reduction of aqueous Cr(VI) under visible-light (λ>420 nm) irradiation. Thus, ZnFe 2 O 4 /CPVC nanocomposites are promising for use as a new efficient visible-light-driven photocatalyst .
研究领域:
材料科学
·
环境化学
·
纳米技术
·
光催化
·
高分子化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Guorong Hu,Jilin Wu,Ke Du,Zhongdong Peng,Ming Jia,Hao Yang,Yanbing Cao
The surface-fluorinated Li 4 Ti 5 O 12 nanowires/reduced graphene oxide composite is synthesized through a hydrothermal procedure. Lithium ion transport is promoted by forming a special morphology of lithium titanate nanowires, meanwhile, electronic transmission is facilitated by surface fluorination and conductive network of graphene coating. These three kinds of synergistic effects greatly improve the rate performance of lithium titanate . The surface-fluorinated Li 4 Ti 5 O 12 nanowires/reduced graphene oxide composite exhibits high specific capacities (167.5 mAh g −1 at 1 C and even 132.6 mAh g −1 at 10 C) and good cyclic stability (95% capacity remain after 300 cycles at 5 C). The influences of surface fluorination and graphene coating on electrochemical performance of lithium titanate are investigated in detail in terms of reversible capacity, cyclability and rate capability. Its excellent electrochemical properties make it become possible to be a potential anode material for high-rate lithium-ion batteries applied in high power facilities.
研究领域:
材料科学
·
电化学
·
纳米科技
·
能源存储
·
锂离子电池
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）