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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Jiahui Xu,Jia-qi Bai,Wenjie Si,Yunhai Zhang,Jiazhao Tan,Mengdie Cai,Qin Cheng,Song Sun
Non-noble metals have attracted worldwide attention for the catalytic hydrogenation of halonitrobenzene due to their high activity, low price, and abundance on Earth. However, the construction of effective and stable non-noble-metal catalysts for the selective hydrogenation of halonitrobenzene to haloaniline by a simple method remains challenging. Herein, we report a facile one-pot method for the synthesis of N,S-co-doped mesoporous carbon-supported non-noble-metal catalysts through carbonization of a mixture of metallic precursors and 2-aminothiazole in molten ZnCl2. The prepared Co-NSPC catalyst showed excellent activity and selectivity with a turnover frequency of 84.4 h–1 in the hydrogenation of p-chloronitrobenzene to p-chloroaniline. Furthermore, Co–Nx was found to be the main active site for this reaction on the basis of characterization and experimental data, and the introduction of S promoted the formation of Co–Nx sites. Moreover, the Co-NSPC-800 catalyst can be reused at least four times and applied to the hydrogenation of 10 kinds of halogenated nitrobenzenes with excellent selectivity.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2019
·
IF 12.221
Jiaojiao Zhao,Yurong He,Fei Wang,Wentao Zheng,Chunfang Huo,Xi Liu,Haijun Jiao,Yong Yang,Yongwang Li,Xiaodong Wen
For the hydroformylation of alkenes, developing ligand-free heterogeneous catalysts is a research focus because of both fundamental research interests and potential commercial applications. However, the leaching of active metals (e.g., Co, Rh) during the hydroformylation reaction seriously hinders the development of heterogeneous catalysts. Suppressing metal leaching with the use of an effective protectant is a possible solution to this problem. In this work, Co leaching was suppressed by the addition of suitable protectants (e.g., citric acid, oxalic acid, and formic acid), thus providing a stable heterogeneous catalytic system. In situ Fourier transform infrared proved that toluene and 1-hexene can promote the solvation of Co carbonyls because of the solvent effect. In contrast, formic acid can be converted to formate species (HCOO) on the surface of Co and effectively suppress the formation of Co carbonyls. Theoretical calculations further proved that high CO coverage on the surface of Co leads to the formation of Co carbonyl species. Furthermore, carboxyl radicals resulting from the dissociation of the O–H bonds of organic acids exhibit strong adsorption on the surface of Co. The intrinsic role of the protectants in suppressing metal leaching is attributed to the decreased CO coverage on the surface of Co by competitive adsorption.
研究领域:
催化
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化学工程
·
无机化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Mingyao Yang,Yanwei Li,Jinhuan Yao,Jiqiong Jiang,Xuejiao Chen,Wenhan Xu
Prussian blue (PB) and its analogs (PBAs) have become a research hotspot in the fields of electrochemical energy storage and electrochromism due to their good reversible redox activity, and reversible color change response in different redox states. Herein, a series of trimetallic PBAs (Co/NiHCF with Co to Ni molar ratios of 1:0, 3:1, 1:1, 1:3, and 0:1) are synthesized by a facile co-precipitation method. In particular, the impact of Co to Ni molar ratio on the lithium storage and electrochromic properties of Co/NiHCF materials are systemically investigated. All five samples possess good crystallinity but the particle size decreases with the reduction of Co/Ni molar ratio. The color change, redox reaction potential, and lithium storage activity of the samples can be readily controlled by adjusting the molar ratio of Co to Ni. The lithium storage activity of the samples strengthens with the increase of Ni content in Co/NiHCF, accompanied by a decrease in redox potentials. With the increase of Ni content, the color of the Co/NiHCF film in the oxidation state changes from purple-red to orange, and finally to yellow; in the reduction state, the color of the film changes from green to light green and then to colorless. All the samples exhibit superior rate capability, excellent cycling stability, and short switching time (in the range of 1.6 to 4.3 s). The present work demonstrates a facile strategy for readily tunning the lithium storage activity, redox reaction potentials, and realizing rich color changes of PBA-based bifunctional materials.
研究领域:
电化学
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材料科学
·
能源存储
·
电致变色
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Changming Zhang,Zhihao Liu,Yongjin Zou,Fen Xu,Lixian Sun,Zhicong Hu,Sensen Yu,Cuili Xiang
Spinel-type materials are attracting great attention as potential electrocatalysts for the hydrogen- and oxygen-evolution reactions. However, their inherent catalytic activities are not on par with those of precious-metal catalysts, and their poor stabilities continue to constrain their rapid development. In this study, we fabricated Zr-CuCo 2 S 4 nanowires and Co(OH) 2 nanosheet–nanowires using electrochemical methods, resulting in lattice defects, sulfur vacancies, and more exposed active sites that catalyze the hydrogen- and oxygen-evolution reactions. DFT calculations revealed that sulfur vacancies enhance intrinsic activity, while Zr doping reduces the energy barrier for H*–OH* adsorption, promotes the formation of additional sulfur vacancies, and modulates active-site Cu/Co valence states, which greatly enhances water-dissociation and H*-adsorption kinetics. Consequently, Zr-CuCo 2 S 4 /Co(OH) 2 requires low overpotentials of 88 and 208 mV, respectively, to support highly stable alkaline hydrogen- and oxygen-evolution reactions at 10 mA cm −2 . This study provides a rational strategy for designing low-cost spinels for green and clean energy.
研究领域:
材料科学
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电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Hu Yang,Chang Li,Linzhe Lü,Zhuogen Li,Shiqi Zhang,Zheng Huang,Rui Ma,Sisi Liu,Ming Ge,Wei Zhou,Xiaolei Yuan
Although Platinum (Pt)-based alloys have garnered significant interest within the realm of direct methanol fuel cells (DMFCs), there still exists a notable dearth in the exploration of the catalytic behavior of the liquid fuels on well-defined active sites and unavoidable Pt poisoning because of the adsorbed CO species (CO ads ). Here, we propose an electronegativity-induced electronic redistribution strategy to optimize the adsorption of crucial intermediates for the methanol oxidation reaction (MOR) by introducing the Co element to form the PtCo alloys. The optimal PtCo hollow nanospheres (HNSs) exhibit excellent high-quality activity of 3.27 A mg Pt −1 , which is 11.6 times and 13.1 times higher than that of Pt/C and pure Pt, respectively. The in-situ Fourier transform infrared reflection spectroscopy validates that electron redistribution could weak CO adsorption, and subsequently decrease the CO poisoning adjacent the Pt active sites. Theoretical simulations result show that the introduction of Co optimize surface electronic structure and reduce the d-band center of Pt, thus optimized the adsorption behavior of CO ads . This study not only employs a straightforward method for the preparation of Pt-based alloys but also delineates a pathway toward designing advanced active sites for MOR via electronegativity-induced electronic redistribution.
研究领域:
材料科学
·
纳米技术
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催化
·
能源材料
·
燃料电池技术
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表面化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yahui Wang,Xuandong Li,Xijiang Han,Ping Xu,Liru Cui,Honghong Zhao,Dawei Liu,Fengyuan Wang,Yunchen Du
Transition metal carbides with good chemical stability and moderate dielectric constants are becoming popular electromagnetic (EM) absorption materials. In this work, Mo 2 C/Co/C composites, a ternary loss system (conductivity loss, polarization loss, and magnetic loss) for EM absorption, have been successfully fabricated by rationally regulating the growth of ZIF-67 on the surface of MoO 3 nanorods and subsequent pyrolysis process. The chemical compositions of Mo 2 C/Co/C composites indeed play a dominant role in tailoring their EM functions. It is revealed that conductivity loss, polarization loss, and magnetic loss are together responsible for the attenuation of EM energy. Although the involvement of Mo 2 C nanoparticles weakens magnetic loss capability to some extent, there will be a positive reinforcement in conductivity loss through the synergistic effects among different components. In addition, Mo 2 C nanoparticles can further provide considerable dipole orientation polarization and interfacial polarization. Among these ternary composite, MCC-50 with 30.9% of carbon, 53.6% of Mo 2 C, and 15.5% of Co, exhibits the best EM absorption performance, whose reflection loss intensity and qualified response bandwidth are superior to those of most carbide-based composites in previous studies. These results suggest that the rational integration of components with different loss mechanisms will be an effective pathway to enhance EM absorption.
研究领域:
材料科学
·
电磁学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 152
·期 12
·3843-3852
·
IF 2.936
Huang Xuehui,Yang Na,Li Xiaobo,Pan Hongyun,Song Xiaozhan,Chang Yu
La 0.8 Sr 0.2 MnO 3 (LSM) catalyst has been successfully prepared by solid phase method (G-LSM-T), sol–gel method (C-LSM-T) and molten salt method (S-LSM-T), using as-prepared MnCO 3 microspheres as templates, respectively. It was shown that the S-LSM-550 catalyst presented well-formed perovskite structures, large specific surface area (49.65m 2 /g) and promising catalytic activity in CO oxidation, which T 50 and T 90 for CO conversion over fresh S-LSM-550 were 145.14 °C and 170.73 °C. The S-LSM-550 calcined at 550 °C for 2 h exhibited excellent thermal stability and catalytic activity compared with the samples prepared by solid phase method and sol–gel method. Its superior catalytic performance could be greatly attributed to its stable microstructure, high surface Mn 4+ /Mn 3+ molar ratio and more available surface adsorbed oxygen species. Graphical Abstract
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2018
·
IF 4.244
Quan Wang,Shigang Shen
A novel porous monolithic column was synthesized via in situ free-radical polymerization within a stainless steel column (50 × 4.6 mm i.d.) by using triallyl isocyanurate and methyl methacrylate as co-monomers, ethylene glycol dimethacrylate as a crosslinking agent, 1,4-butanediol, 1- dodecanol , and N, N-dimethylformamide as tri-porogens, and azobisisobutyronitrile as an initiator. The optimized monolithic columns were investigated by scanning electron microscopy, a nitrogen absorption-desorption apparatus, and mercury intrusion porosimetry. The effect of mobile phase composition and temperature on chromatographic behavior was studied in detail as well. The results showed that homemade monolithic columns not only have relative uniform porosity structure, low back pressure, and high thermal stability, but also show high column efficiency, the theoretical plates number of the new polymer monolithic column exceeded 31,000 plates m −1 . Good resolution was achieved for HPLC separation of small molecules, including polycyclic aromatic hydrocarbons , isomers of phenols, and the Chinese herbal medicine notoginseng. Methodological validation of six drugs in notoginseng show that correlation coefficients of the linear regressions were in the range of 0.9989–0.9997; the value of relative standard deviation for precision were in the range of 1.37–4.21% for intra-day and 0.34–5.31% for inter-day, respectively; the values of accuracy expressed by recovery were in the range of 100.57–102.51%, 95.18–102.68%, 101.61–102.82%, 100.94–102.40%, 100.99–103.15% and 99.49–103.91% for the six drugs in order, respectively. Taking aromatic hydrocarbons as samples, the relative standard deviation values of the run-to-run (n = 5) and column-to-column (n = 5) based on peak area were < 2.01% and 2.39%, and two RSDs based on retention time were < 2.56% and 2.23%, respectively. The result showed that the polymer monolithic column has good separation ability and high permeability for small molecular substances.
研究领域:
分析化学
·
药学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Atian Xie,Jiuyun Cui,Jin Yang,Chunxiang Li,Yi Wang,Jiangdong Dai
The effective treatment of oily wastewater is of great significance for the protection of the ecological environment and human health. Aiming to prepare a membrane with excellent antifouling properties, a new active antifouling carbon cloth@Ni-Co LDH/Ag (CC@LDH/Ag) membrane was reported here via in situ hydrothermal growth and followed photo-deposition methods. The effects of Ag deposition on self-cleaning ability and surface wettability of CC@LDH/Ag membrane were studied. The experimental results showed CC@LDH/Ag membrane is superhydrophilic/underwater superoleophobic, and exhibited high separation efficiency (>98.6%) and high flux (6551–22,050 L m −2 h −1 ) for different kinds of oil/water mixtures. Moreover, CC@LDH/Ag membrane also displayed excellent environmental and mechanical durability. Good self-cleaning ability enabled CC@LDH/Ag membrane to be separated at least 30 times, and still maintained high separation performance. The self-cleaning CC@LDH/Ag membrane may hold great application prospects in oily wastewater remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ISIJ INTERNATIONAL
·
2017
·Vol. 57
·期 1
·62-67
·
IF 1.11
Zijian Su,Yuanbo Zhang,Yingming Chen,Guanghui Li,Tao Jiang
A considerable amount of works were focused on the formation mechanism of calcium ferrite phases during the iron ore sintering process, especially under various O2 content atmospheres at temperatures higher than 1100°C. But little attention has been paid on reactions between CaO and iron oxides in CO–CO2 atmospheres at lower temperatures. In this study, the solid state reaction mechanisms between CaO and Fe3O4 under CO–CO2 atmospheres at 800°C–1100°C were revealed by using XRD, VSM, etc. The results indicated that Ca2Fe2O5 was easily formed under 5–50 vol% CO/(CO+CO2) atmosphere above 850°C via the reaction of 6CaO + 2Fe3O4 +CO2 = 3Ca2Fe2O5 + CO and the reaction would be promoted with increasing the roasting temperature. In the CO–CO2 atmosphere, Fe3O4 is easily oxidized to Fe2O3 in the presence of CaO because CO2 components act as oxidative medium for the oxidation of Fe2+ to Fe3+.
研究领域:
冶金学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Caihong Fang,Xiaomin Jiang,Jinwu Hu,Jiaojiao Song,Na Sun,Deliang Zhang,Long Kuai
Ruthenium nanocrystals with small size and special morphology are of great interest in various catalytic reactions due to their high activities. However, it is still a great challenge to downsize these nanocatalysts to a sub-nano scale (<2 nm). Herein, we reported a synthesis of ultrasmall size and uniform Ru nanoparticles through a rapid one-pot method. The prepared Ru nanocrystal shows a wormlike shape, in which the diameter is as thin as 1.6 ± 0.3 nm and the length is 13.6 ± 4.4 nm. These Ru nanoworms (NWs) are quite steady during the synthetic process even though the reaction time was further prolonged. We also examined their catalytic activity toward CO oxidation by loading Ru NWs on TiO2 to form Ru NWs/TiO2 catalysts. These catalysts exhibit a high activity of 100% CO conversion at 150 °C, which is much lower than the normal Ru NPs/TiO2 nanostructures. Based on our detailed investigations, we proposed that the small size, special morphology, and TiO2 support are the keys for their significantly improved catalytic activity. We believed that these reasonable discoveries provide a methodology and opportunity to get highly active catalysts for CO oxidation by a detailed increase in their active sites.
研究领域:
材料科学
·
催化化学
✓ 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）