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ACS Applied Materials & Interfaces · 2020 · IF 8.758

MOF-Templated Preparation of Highly Dispersed Co/Al2O3 Composite as the Photothermal Catalyst with High Solar-to-Fuel Efficiency for CO2 Methanation

Xi Chen,Qiang Li,Meng Zhang,Juanjuan Li,Songcai Cai,Jing Chen,Hongpeng Jia

CH4 production from CO2 hydrogenation provides a clean approach to convert greenhouse gas CO2 into chemical energy, but high energy consumption in this reaction still restrains its further application. Herein, we use a light-driven CO2 methanation process instead of traditional thermocatalysis by an electrical heating mode, with the aim of greatly decreasing the energy consumption. Under UV–vis–IR light irradiation, the photothermal CO2 methanation over highly dispersed Co nanoparticles supported on Al2O3 (Co/Al2O3) achieves impressive CH4 production rates (as high as 6036 μmol g–1 h–1), good CH4 selectivity (97.7%), and catalytic durability. The high light-harvesting property of the catalyst across the entire solar spectrum coupled with its strong adsorption capacity toward H2, CO2, CO, and abundant active sites are proposed to be responsible for the better photothermocatalytic performance of Co/Al2O3. Furthermore, a novel light-promotion effect is also revealed in CO2 methanation, where UV–vis light irradiation induces oxygen vacancies and improves the proclivity toward adsorption of H2, CO2, and CO, finally resulting in a significant enhancement of the photothermocatalytic activity for CH4 production. By concentrating the low-intensity light (120 mW/cm2) via a Fresnel lens, a photothermal CO2 conversion efficiency of more than 50% with a good CH4 selectivity (76%) is achieved on the optimal catalyst under a dynamic reaction system, which indicates the bright prospect of photothermal CO2 methanation.

研究领域: 化学工程 · 能源科学 · 环境科学
✓ 已验证 DOI PubMed 高影响因子
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2021 · IF 4.539

Peroxidase-like and oxidase-like nanozyme activities of reusable Mn–Co–S–Se/Ni foam for antibacterial application

Yumeng Lian,Yi Wang,Dun Zhang,Likun Xu

Developing a stable and reusable material for antibacterial application in an enzyme-like system is still a challenge. Herein, Mn–Co–S–Se (MnCo 2 S x Se 4–x )/Ni foam (NF) are synthesized by introducing S 2– and Se 2– in MnCo 2 O 4 /NF with a facile hydrothermal approach. With the different molar ratios of S/Se, the surface morphology of MnCo 2 S x Se 4–x /NF shows different growth and the catalytic activity also presents regular changes. MnCo 2 S 3.1 Se 0.9 /NF possesses a high enzyme-like ability with higher V max than natural horseradish peroxidase . Due to the outstanding peroxidase-like activity, MnCo 2 S 3.1 Se 0.9 /NF also exhibits broad-spectrum bactericidal performance towards Escherichia coli and Staphylococcus aureus which stems from the formation of ·O 2 – from H 2 O 2 . In the reutilization experiment, the enzyme-like activity keeps a stable value after 25 cyclic tests and the bactericidal performance is still stable after 10 cyclic tests, proving that MnCo 2 S 3.1 Se 0.9 /NF possesses relative stability and reusability. This research showed the great prospect of new energy and environmental catalysis.

研究领域: 生物材料学 · 环境催化 · 纳米酶研究
✓ 已验证 DOI 高影响因子
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Nanoscience and Nanotechnology Letters · 2017 ·Vol. 9 ·期 6 ·867-872 · IF 1.889

Electrocatalytic Activity of Hierarchically Nanoporous Au@Ti–SiO2/Ni–W–Co Composite Electrode for Hydrogen Evolution

Du Jingjing,Song Ya,Feng Yahui,Li Na,Tan Haihu,Li Changyun,Xu Lijian

Hierarchically nanoporous Ti–SiO2 particles were synthesized by dissolving template method, and the hierarchically nanoporous Au@Ti–SiO2 particles were further prepared by in-situ synthesis method using NaBH4 as reducing agent. The components of the hierarchically nanoporous Au@Ti–SiO2 particles and Ni–W–Co alloy electrode were investigated by energy dispersive spectrometer (EDS). In addition, the hierarchically nanoporous Au@Ti–SiO2/Ni–W–Co composite electrode was fabricated by the method of composite electrodeposition using hierarchically nanoporous Au@Ti–SiO2 particles as composite nanoparticles. Finally, the electrocatalytic activities for hydrogen evolution of different electrodes were investigated. Results showed that, the mass fractions of Ni, W and Co were 62.78%, 11.75% and 25.47% respectively in the coating of Ni–W–Co alloy electrode. The mass fractions of Au and Ti were 0.94% and 4.21% respectively in the hierarchically nanoporous Au@Ti–SiO2 particles which indicated that the Au nanoparticles were successfully doped into the hierarchically nanoporous Ti–SiO2 particles. And the results of electrocatalytic activity study showed that, Co and W have good electrocatalytic activity for hydrogen evolution, which can greatly improve the electrocatalytic activity for hydrogen evolution. The electrocatalytic activity of Ni–W–Co alloy electrode was superior than that of Ni electrode and Ni-Walloy electrode. The electrocatalytic activity for hydrogen evolution of hierarchically nanoporous Au@Ti–SiO2/Ni–W–Co composite electrode was improved because of adding Au@Ti–SiO2 and reached the optimal value when the concentration of nanoporous Au@Ti–SiO2 particles was 1.6 g/L.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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Frontiers of Chemical Science and Engineering · 2021 ·Vol. 16 ·期 4 ·443-460 · IF 4.204

Carbon-coated Ni-Co alloy catalysts: preparation and performance for in-situ aqueous phase hydrodeoxygenation of methyl palmitate to hydrocarbons using methanol as the hydrogen donor

Shi Yinteng,Ai Lin,Shi Haonan,Gu Xiaoyu,Han Yujun,Chen Jixiang

Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d -band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n -pentadecane and n -C 6 - n -C 16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO 2 recovered the catalyst reactivity.

研究领域: 化学工程 · 催化材料科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY · 2024 ·Vol. 110 ·期 1 ·103-117 · IF 2.3

Novel La1-xMxCo0. 5Ni0. 5O3 perovskite with low CO selectivity for enriched hydrogen production from methanol reforming for HT-PEMFCs application

Chen Gaokui,Shen Qiuwan,Zhang Xin,Zhao Tianyun,Huang Naibao,Li Shian

Abstract Methanol steam reforming (MSR) is considered as an effective way to provide on-line hydrogen production technology for fuel cell applications, and perovskite catalyst is considered as an efficient and potential catalyst for this technology. A series of La 1-x M x Co 0.5 Ni 0.5 O 3 perovskite catalysts doped with yttrium(Y) and cerium(Ce) at A site were prepared by sol-gel method. The catalysts were characterized by SEM, EDS, BET, XPS and XRD techniques. The results of XRD, SEM and BET show that the main phase of the catalyst is perovskite when a small amount of Y or Ce is doped. However, with the increase of Y and Ce doping levels, some other new phases appeared. The appearance of the new phase of yttrium oxide promotes the richer pore structure of the catalyst, increases the pore volume and pore diameter, and enhances the active catalytic sites. More importantly, it also promotes the increase of the specific surface area, allowing the active component particles to maintain a very uniform dispersion state, effectively preventing the aggregation of active components and improving the catalytic activity. From the XPS results of Y-doped catalyst with x of 0.9, Y-O bonds belonging to Y 2 O 3 can be observed, the presence of yttrium carbonate species can promote the formation of oxygen vacancies, thereby accelerating the catalytic reaction and enhancing the catalytic performance. After multiple cycles of start-stop stability experiments, the results showed that the CO selectivity of the gas product was 1.8% and remained unchanged without significant fluctuations. The novel yttrium-doped catalyst with x of 0.9 developed in this study is a potential catalyst which can directly provide hydrogen-rich source for HT-PEMFCs applications. Graphical Abstract The novel La 0.1 Y 0.9 Co 0.5 Ni 0.5 O 3 catalyst, with high specific surface area and well-developed pore structure, exhibits excellent low CO selectivity and stability in the MSR process, which can be a promising catalyst for directly providing hydrogen-rich source for HT-PEMFCs applications.

研究领域: 化学工程 · 催化材料 · 能源科学
✓ 已验证 DOI 高影响因子
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Catalysis Science & Technology · 2022 ·Vol. 12 ·期 20 ·6285-6293 · IF 6.177

Highly dispersed Co-N-RGO electrocatalyst based on an interconnected hierarchical pore framework for proton exchange membrane fuel cells

Jie Lian,Qiang Bai,Jinyu Zhao,Xiaomin Wang

It is a grand challenge to develop non-noble metal-based oxygen reduction (ORR) catalysts with relatively high activity and stability for proton exchange membrane fuel cells (PEMFCs). Herein, zeolitic imidazolate framework (ZIF) precursors were grown in situ on graphene oxide (GO), and Co-N-RGO catalysts with good stability were successfully prepared. Density functional theory (DFT) calculation results show that Zn and Co are mixed and alternated to form a Zn-Co-ZIF structure instead of forming ZIF-8 or ZIF-67, separately. Such a combination promoted the uniform distribution of Co atoms in the N-doped carbon frameworks during subsequent heat treatment. By means of accurate adjustment of the molar ratio of Co/Zn species in the Zn-Co-ZIF precursors, the hierarchical porous structure connected with uniformly dispersed Co–Nx sites was established after thermal activation, and the utilization rate of active sites was improved. The RGO in catalysts, connecting each derivative carbon particle, formed a connected network and reduced the ohmic impedance of the catalyst layer. This strategy avoided the traditional tedious steps of additional acid-leaching and second heat treatments. What's more, the ORR performance of the Co-N-RGO samples was evaluated. The catalyst exhibited a positive half-wave potential (0.75 V vs. RHE), high limiting diffusion current density, and positive stability at 0.5 M H2SO4. Meanwhile, the H2/O2 fuel cell test result displayed a relatively high ORR activity with a peak power density of 334 mW cm−2.

研究领域: 能源材料 · 电化学 · 纳米材料 · 催化化学 · 燃料电池技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Self-supported Co-Ni-S@CoNi-LDH electrode with a nanosheet-assembled core-shell structure for a high-performance supercapacitor

Yu Zhang,Wangfeng Cai,Yajie Guo,Yan Wang

In this work, a nanosheet-assembled core-shell structure composite of Co-Ni-S@CoNi-LDH was prepared on Ni foam via hydrothermal synthesis , in which Co-Ni-S nanowires as cores were assembled with the shell of CoNi-LDH nanosheets. The combination of the high conductivity of Co-Ni-S, the high specific surface area of CoNi-LDH and the multivalent state of Ni and Co provided more active sites, short and effective ion transport paths, and great synergy, which played significant roles in the excellent performance of Co-Ni-S@CoNi-LDH. Meanwhile, the nanosheet-assembled core-shell structure improved the overall stability. Based on the characterisation and the performance measurements, the Co-Ni-S@CoNi-LDH electrode showed an excellent electrochemical performance. The Co-Ni-S@CoNi-LDH electrode acquired a specific capacitance of 2414 F/g at a 1 A/g current density and a high cycle stability with an 89.7% retention after 3000 cycles. The assembled hybrid supercapacitor Co-Ni-S@CoNi-LDH//AC delivered a high energy density of 59.11 Wh kg −1 at an 855.43 W kg −1 power density, as well as an excellent rate performance of 81% after 5000 cycles at a 5 A/g current density, showing good potential for practical applications.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Synthesis of a Co–Sn Alloy-Deposited PTFE Film for Enhanced Solar-Driven Water Evaporation via a Super-Absorbent Polymer-Based “Water Pump” Design

Yuzhu Wang,Le Zhao,Feng Zhang,Kai Yu,Chunyu Yang,Jingjing Jia,Wei Guo,Jingxiang Zhao,Fengyu Qu

Solar-driven water evaporation is a promising solution to water pollution, the energy crisis, and water shortages. However, the approach in which the photothermal film is in direct contact with bulk water for water evaporation may lead to a large amount of heat loss, thereby reducing the light-to-heat conversion efficiency (η) of the photothermal film. Here, a highly efficient solar-driven water evaporation system was developed using a Co–Sn alloy-deposited Teflon (PTFE) film (Co–Sn alloy@PTFE) and super-absorbent polymers (SAPs) supported with a floating foam substrate. The Co–Sn alloy with full-spectrum (200–2500 nm) absorption characteristics is devoted to high light-to-heat conversion, while the porous PTFE with high mechanical performance can support the Co–Sn alloy. We used density functional theory to prove that the Co–Sn alloy had a strong adhesive force with PTFE without surfactants due to the high adsorption energy between the (101) crystal plane of the Co–Sn alloy and the hydroxyl group on the PTFE film. Importantly, via the SAP-based “water pump” design, we improved the η of the Co–Sn alloy@PTFE film to 89%, mainly because the SAP not only effectively performed water transportation but also markedly reduced the heat loss of the Co–Sn alloy@PTFE film. Our work highlights the strong potential of Co–Sn alloy@PTFE-based light-to-heat conversion systems for realizing highly effective solar energy-driven water evaporation.

研究领域: 材料科学 · 环境科学 · 能源科学
✓ 已验证 DOI PubMed 高影响因子
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CRYSTENGCOMM · 2020 ·Vol. 22 ·期 23 ·4005-4013 · IF 3.117

Engineering CuOx–ZrO2–CeO2 nanocatalysts with abundant surface Cu species and oxygen vacancies toward high catalytic performance in CO oxidation and 4-nitrophenol reduction

Baolin Liu,Yizhao Li,Shaojun Qing,Kun Wang,Jing Xie,Yali Cao

Highly dispersed surface Cu species and oxygen vacancies are important for CuOx–CeO2 catalysts in many reactions, but it is difficult to increase the concentrations of highly dispersed Cu species and oxygen vacancies simultaneously by only adding a Cu component. Herein, CuOx–ZrO2–CeO2 (CZC) nanocatalysts with different ratios of Cu/Zr have been effectively produced by a simple solvent-free synthetic strategy. The effect of Zr doping on the structure and reactivity of the CuOx–CeO2 catalysts has been investigated with the help of carbon monoxide (CO) oxidation and 4-nitrophenol (4-NP) reduction as model reactions. It is revealed that the introduction of Zr relieved the agglomeration of surface Cu species, produced more oxygen vacancies in the interior and Cu+ species on the surface of the catalyst, and increased the reducibility of CuOx–CeO2. The CZC catalysts show remarkably enhanced catalytic activity due to the abundant surface active sites and the improved redox properties provided by the suitable doping of Zr into CuOx–CeO2. This work not only offers a practicable way to reconstruct the distribution of active metals on the metal oxide support but also provides a high-efficiency strategy to prepare oxide catalysts with excellent catalytic performance.

研究领域: 催化化学 · 材料科学
✓ 已验证 DOI 高影响因子
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NANOTECHNOLOGY · 2021 ·Vol. 32 ·期 34 ·345702 · IF 3.874

Regulating the core/shell electric structure of Co3O4@Ni–Co layered double hydroxide on Ni foam through electrodeposition for a quasi-solid-state supercapacitor

Yuqiang Zhang,Yan Wang,Jiahui Zhu,Xubin Zhang,Wangfeng Cai

A flower-like structured electrode material of Co3O4@Ni–Co layered double hydroxide (LDH) grown on Ni foam (Co3O4@Ni–Co LDH/NF) was prepared via an in situ growth, annealing and electrodeposition process. The Co3O4@Ni–Co LDH/NF electrode was prepared with the optimized conditions of annealing temperature 300 °C, deposition time 20 min and Ni/Co ratio 1:1. The results showed that the as-prepared electrode material exhibited an excellent specific capacitance and great cycling stability. Furthermore, an quasi-solid-state supercapacitor was assembled using the prepared Co3O4@Ni–Co LDH/NF as the positive electrode and activated carbon on Ni foam (AC/NF) as the negative electrode. The as-assembled device presented a high energy density and power density.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF APPLIED POLYMER SCIENCE · 2022 ·Vol. 139 ·期 38 ·e52918 · IF 3.057

Superior stretchable and tough P(AA-co-AAm)/silica hybrid hydrogels enabled by acid-mediated radiation polymerization

Yukun Tian,Yongzhi Hong,Yunlong Wang,Yuan Tian,Zhihao Wang,Meixing Ai,Jun Ma

The emerging stretchable and tough hydrogels find their extraordinary contributions in widespread use. However, the applicability of existing tough hydrogels in harsh environments like highly acidic stomachs has remained a challenge. Here, we develop superior stretchable and tough P(AA -co- AAm)/SiO 2 hybrid hydrogels through radiation-induced polymerization and crosslinking in the presence of acids. The performance of the nanocomposite gels was optimized by altering fabrication variables including acid concentration, monomer composition and absorbed dose. The mechanic tests show that the protonated hybrid hydrogels displayed a high elongation at break (1919%), fracture strength (117 kPa), and compressive strength at 50% strain (126 kPa). These values are superior to those of conventional polyelectrolyte hydrogels and expect to significantly broaden the application. The proposed strategy is quite general and offers an alternative strategy to develop tough hydrogels.

研究领域: 材料科学 · 高分子化学 · 生物医学工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF APPLIED POLYMER SCIENCE · 2017 ·Vol. 135 ·期 11 ·45984 · IF 1.86

Synthesis and properties of non-cytotoxic poly(l-malic acid acetate-co-l-lysine ester)s with thermo-sensitivity as hydrophobic drug nanocarrier

Ying Yue,Zhihui Fan,Chang Zheng,Lan Ding,Huiying Wang,Miao Zhang,Kuilin Deng

In this investigation, a group of poly( l -malic acid acetate- co - l -lysine ester)s (PMALs) with excellent thermo-sensitivity and non-cytotoxicity were prepared by an optimized synthetic route from natural l -malic acid and l -lysine. The structure and properties of PMALs including monomers were systematically characterized by FTIR, 1 H NMR, UV, gel permeation chromatograph, scanning electron microscope, contact angle measurement, cell counting kit assess (CCK-8), and confocal laser scanning microscopy (CLSM). Three PMALs show a reversible lower critical solution temperature of 8–36 °C depending on their chemical structure. The contact angle measurement revealed a considerable discrepancy in the hydrophilicity/hydrophobicity of PMALs and further influence on their thermo-sensitivity. The viability of HeLa cells exposed to 0.2–100 μg/mL PMALs solution was found to be in a range 80–103% after 24, 48, and 72 h of incubation, indicating no cytotoxicity. Moreover, a spherical nanocarrier with core-shell structure was facilely fabricated via the thermo-sensitivity of PMALs and hydrophobicity of drug. CLSM observations manifested that the hydrophobic-curcumin-enwrapped nanocarriers can clearly internalize into the cellular inside. The sustained release of curcumin from nanocarriers in vitro provided a possibility of depressing fast hydrolytic degradation at physiological pH or other side-effects. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 45984.

研究领域: 生物材料学 · 药物递送系统 · 高分子化学
✓ 已验证 DOI 高影响因子
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