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FUEL · 2022 · IF 8.035

Ultrafine Co-MoS2 monolayer catalyst derived from oil-soluble single-molecule polyoxometalates for slurry phase hydrocracking

Yanfei Chen,Yukun Lu,Zekun Guan,Shoujie Liu,Chao Feng,Guangxun Sun,Jilei Liang,Yuan Pan,Chenguang Liu,Yunqi Liu

Herein, a novel single-molecule confinement-sulfurization strategy was proposed to construct ultrafine Co-MoS 2 monolayer catalysts by using oil-soluble single-molecule polyoxometalates (POMs), (DODA) 6 Co 2 Mo 10 , as precursors. Well-defined Co 2 Mo 10 -POM, acting as molecular pre-assembling platform, is introduced for the atomically precise construction of bimetallic sites. Highly efficient conversion of VR under severe condition is realized with (DODA) 6 Co 2 Mo 10 . The origin of prominent catalytic performance can be attributed to the in-situ formation of ultrafine single-layered Mo-based nanosheets with abundant exposed CoMoS active sites. By combining synchrotron radiation-based X-ray absorption spectroscopy and density functional theory calculations, we further discover that there is clearly intimate interaction between Mo and Co atoms and the dissociation of molecular hydrogen at CoMoS phases is energetically preferred, leading to remarkable hydrogenation and coke suppression activity. This work highlights an idea on the rational design and targeted synthesis of ultrafine bimetallic catalysts for slurry phase HCK with dramatically synergistic catalysis.

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 ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Realization of grain growth and suppressed bulk defects for efficient solution-processed Cu2ZnSn (S, Se)4 solar cells via co-doping strategy

Chang Miao,Meiling Ma,Yingrui Sui,Yue Cui,Zhanwu Wang,Lili Yang,Fengyou Wang,Xiaoyan Liu,Bin Yao

Environmentally benign and earth-abundant constituent’s kieserite Cu 2 ZnSn (S, Se) 4 (Cotises) is considered as a hopeful photovoltaic material. Unfortunately, the severe tail state caused by various harmful deep defects in CZTSSe absorber prevents further development of its device efficiency. Here, we report firstly that the Co was incorporated into CZTSSe films to form the Cu 2 Co x Zn 1-x Sn (S, Se) 4 (CCZTSSe) films using a two-step annealing and solution-processing technique method. Through optimized the Co/(Co+Zn) ratio, the CCZTSSe film has excellent good surface morphology and single-phase composition. Appropriate amount of Co elements replacing Zn elements in CZTSSe films can effectively reduce the degree of Cu-Zn disorder, thus inhibiting [2Cu Zn +Sn Zn ] defect clusters and Cu Zn defects. The detrimental deep defects located in the film were effectively passivated to reduce electrostatic potential fluctuations, resulting in relief of the trailing state. Therefore, a champion device having an efficiency of 7.50 % with a fill factor (FF) of 61.00 % was achieved from CCZTSSe with 3 % Co content. This work provides new insights into the impacts of Co doping in CZTSSe by a solution processed method and offers a deeper comprehension of the origin of the efficiency enhancement of CCZTSSe devices.

研究领域: 材料科学 · 能源技术 · 半导体物理
✓ 已验证 DOI 高影响因子
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Surfaces and Interfaces · 2025 · IF 6.3

Pt-Co nano-alloy catalysts with hierarchical core-shell architectures for enhanced dual-function electrocatalytic water splitting

Haotian Li,Hongyi Li,Zicong Yang,Jiayi Xu,Jiangwen Xu,Jinxu Song,Yukun Chang,Hui Song,Xiaoyu Ma,Rui Pan,Shujun Chen

Introducing other non-precious metals and tailoring the structure to develop Pt-based alloy catalysts is a viable strategy to reduce Pt massive consumption, enhance Pt utilization, and improve the performance of electrocatalysts. In this study, a novel kind of Pt-Co nanoframe alloy catalyst with a hierarchical nanostructure and two distinct particle morphologies has been obtained by using a simple synthetic method. The unique multi-level core-shell structure imparts higher intrinsic activity and conductivity to the Pt-Co Core-shell Nano particles (Pt-Co CSNP), facilitating efficient charge transfer and enhancing both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities. At a current density of 10 mA cm -2 , the Pt-Co CSNP demonstrates excellent electrocatalytic performance, exhibiting overpotentials of 14.7 mV for HER in 0.5 M H 2 SO 4 and 200 mV for OER in 1.0 M KOH, which is a significant improvement over the performance of numerous reported catalysts. According to the mass activity calculation, the Pt-Co CSNP exhibit mass activities of 5.55 and 3.17 A mg Pt -1 for HER and OER, respectively. These values are improved by a factor of 22 and 35 times compared with those of commercial electrodes (Pt/C 20 %, RuO 2 ) at the same overpotential. After 300 h of operation, the catalyst shows minimal performance degradation, making it one of the most effective catalysts for dual-function HER/OER catalysis.

研究领域: 材料科学 · 纳米技术 · 电化学 · 能量转换 · 催化
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2018 · IF 5.091

Co-Al nanosheets derived from LDHs and their catalytic performance for syngas conversion

Mingsheng Luo,Shun Xu,Qingyang Gu,Zuoxing Di,Qinglong Liu,Zhijun Zhao

Layered double hydroxides (LDHs) were innovatively employed in this study as catalyst for synthesis gas conversion to chemicals, such as oxygenates. Cobalt-aluminium layered double hydroxides (Co-Al LDHs) was prepared at different temperatures. and lactate was successfully intercalated into the LDHs by ion-exchange method and then the material was further delaminated in water at ambient temperature. The samples were characterized by SEM, TEM and AFM, and separately dispersed nanosheets can be clearly observed. The prepared lamellas were applied in aqueous-phase synthesis gas conversion reaction. The catalysts generated a superior activity of 0.055–0.675  mol CO · mol Co - 1 · h - 1 and greater oxygenated product (acetaldehyde) selectivity (S Oxy  = 75–88%) than conventional cobalt Fisher-Tropsch (FT) synthesis catalysts. Ammonium ion showed some effect of the selectivity of the acetaldehyde. The original research results suggested a promising application of the mono-dispersed ultrathin cobalt-bearing LDHs nanosheets in the aqueous phase syngas conversion to valuable oxygenate products.

研究领域: 催化 · 化学工程 · 材料科学 · 纳米技术
✓ 已验证 DOI PubMed 高影响因子
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ChemCatChem · 2021 ·Vol. 13 ·期 21 ·4610-4617 · IF 5.686

Low-Temperature CO Oxidation over the Pt−TiN Interfacial Dual Sites

Yifei Yang,Linsen Zhou,Jun Chen,Ruizhi Qiu,Yunxi Yao

Graphical Highly dispersed Pt clusters supported on TiN substrates favor the formation of highly reactive dual sites. Molecular O 2 dissociatively adsorbs on the Ti−Ti bridge sites to form titanium oxynitride (TiN x O y ) skin and the oxygen atom binding on Ti sites readily react with the adjacent CO adsorbed on Pt to attain the catalytic cycle. The interfacial synergistic effect between Pt and TiN results in superior performance in the low-temperature CO oxidation. The metal-support interfacial synergistic catalysis allows the competitive reaction steps to occur in close proximity at different sites, thus decreasing the activation barrier and improving the catalytic efficiency. Combining the structural characterization, reactivity assessments and density functional theory (DFT) calculations, it is found that highly dispersed Pt clusters on TiN substrates favor the formation of Pt−TiN interfacial dual sites, which are highly reactive for the low-temperature CO oxidation with an apparent activation energy as low as 38.7 kJ mol −1 , much less than that on the traditional Pt/TiO 2 or Pt/SiO 2 catalysts. At low temperature, the surface sites of Pt are saturated with CO adsorption due to its high adsorption energy and the molecular O 2 dissociatively adsorbs on the Ti sites to form the titanium oxynitride (TiN x O y ) skin with a low barrier of 0.1 eV. The O atoms binding on Ti sites readily react with the adjacent CO molecules adsorbed on the perimeter of Pt clusters to attain a catalytic cycle with a reaction barrier of 0.5 eV. The interfacial synergistic effect between Pt and TiN is the origin of the low temperature CO oxidation activity on the metal-nitride catalysts.

研究领域: 催化 · 材料科学 · 化学工程 · 表面化学
✓ 已验证 DOI 高影响因子
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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
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