ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shenghan Gao,Yuting Luo,Bo Li,Wen Cai,Huai Liu,Rui Zhang,Wenlong Jia,Lincai Peng
Modulating the electronic environment of single-atom metal catalysts is a promising yet challenging strategy to optimize their catalytic performance. Herein, electron-rich Ru single atoms were successfully confined within a CoOx matrix (Ru0.6CoOx) through a simple manual grinding-reduction strategy. The resulting Ru0.6CoOx catalyst demonstrated exceptional catalytic activity for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), affording a nearly quantitative DMF yield with an impressive DMF productivity of 210.2 molDMF·mol–1Ru·h–1 at 160 °C. This productivity outperforms most of the noble metal-based catalysts for DMF production. Notably, Ru0.6CoOx also enabled the efficient conversion of HMF to DMF at a low reaction temperature of 120 °C or using a concentrated HMF solution (up to 20 wt %). Experimental studies combined with density functional theory calculations (DFT) revealed that the electronic interaction between the Ru species and CoOx generates electron-rich Ru single atoms, which serve as active sites to boost the H2 activation. Furthermore, the introduction of single Ru atoms was shown to increase the acidity of Ru0.6CoOx, thereby facilitating the cleavage of the C–OH bond during HMF hydrogenolysis. The boosted H2 activation ability and improved acidity of Ru0.6CoOx contribute significantly to its outstanding catalytic performance. This work provides valuable insights into the preparation of electron-rich single-atom metal catalysts for the catalytic hydrodeoxygenation of biomass-derived chemicals.
研究领域:
催化化学
·
材料科学
·
化学工程
·
生物质转化
·
密度泛函理论（DFT）
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Zhimin Hao,Dapeng Liu,Xintao Zuo,Haohan Yu,Yu Zhang
Modification of three-dimensional (3D) carbon hosts with metal oxides has been considered as advantageous for the formation of Li 2 O-rich solid electrolyte interface (SEI), which can show fast Li + diffusion, and meanwhile alleviate dendrite problems caused by fragility and nonuniformity of native SEIs. However, the lack of convincing experimental evidence has made it difficult to unveil the true origin of oxygen in Li 2 O-rich SEIs until now. Herein, CoO x embedded carbon nanofibers (CNF-CoO x ) are successfully prepared as high-performance Li anode hosts. By employing 18 O isotope labeling, the role of CoO x during SEI evolution is elucidated, revealing that CoO x contributes significantly to Li 2 O formation by delivering oxygen. Benefiting from the rich Li 2 O content, the as-formed SEIs greatly improve the Li + migration kinetics, and therefore, the CNF-CoO x @Li anode can exhibit excellent cycling stability in half, symmetrical, and full cells.
研究领域:
材料科学
·
电化学
·
电池技术
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产品关联
DOI
PubMed
高影响因子
ChemCatChem
·
2025
·
IF 3.9
Tianao Zhang,Haolong Huang,Yunchong Wang,Qianqian Zhao,Rui Han,Qingling Liu
Graphical CoO x /BCN catalyst with dual active sites was successfully synthesized. This catalyst exhibits excellent selectivity (99%) and a cyclic carbonate yield (98%) in the CO 2 cycloaddition reaction with the nucleophilic reagent KI under solvent-free and mild reaction conditions. This catalyst also has good stability and reusability, providing a new direction for the design of high-performance CO 2 cycloaddition catalysts. The carbon dioxide (CO 2 ) cycloaddition reaction provides an efficient route to achieve resource utilization of CO 2 . However, the inherent chemical stability of CO 2 itself hinders its efficient transformation into cyclic carbonates. Herein, the CoO x /BCN catalyst was successfully prepared by a simple deposition method. The CoO x /BCN exhibited excellent catalytic performance in the CO 2 cycloaddition reaction synergistically catalyzed with the nucleophilic reagent KI under solvent-free and mild reaction conditions (80 °C, 0.8 MPa, 6 h). The yield of cyclic carbonate was 98% and the selectivity was 99%, which was significantly superior to CoO x /CN catalyst (with a cyclic carbonate yield of 73.7%). Furthermore, after six cyclic reactions, CoO x /BCN still maintained a yield of over 93%. It was found that after boron (B) was doped into graphitic carbon nitride (g-C 3 N 4 ), the generated ─NB(OH) 2 group on CoO x /BCN effectively activated the epoxide. Importantly, the interaction between B-doped g-C 3 N 4 and CoO x induced the generation of abundant oxygen vacancies, which provided sufficient active sites for CO 2 adsorption and activation. In addition, carbonates were identified as the main reaction intermediates by in situ DRIFTS, and the possible reaction pathways of the CoO x /BCN catalyst were proposed. Therefore, this work provides new idea for the design of catalysts for CO 2 cycloaddition.
研究领域:
催化
·
二氧化碳利用
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材料科学
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化学反应工程
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xiaoxi Yu,Xiaocui Wu,Fang Guo,Jingping Liu,Qingshan Zhao
As a promising advanced oxidation process , photo-assisted peroxymonosulfate (PMS) activation for wastewater treatment has attracted widespread attentions. However, rational design of synergetic and recyclable catalysts for PMS photo-activation remains a big challenge. In this study, a carbon layer-coated amorphous CoO x supported on graphitic carbon nitride (CoO x @C/g-C 3 N 4 ) composite was fabricated to drive visible-light-assisted activation of PMS for efficient organic pollutant degradation. Amorphous CoO x nanoparticles were in-situ grown on two-dimensional g-C 3 N 4 substrate, among which a carbon layer serves as a high-speed electron transmission channel, facilitating the separation of photogenerated electron-hole pairs and accelerating the Co 3+ /Co 2+ redox cycle. Simultaneously, the carbon layer provides a protective film to suppress Co leaching, thereby improving the catalytic activity and reusability. Owing to the unique heterostructure and synergetic effect, the optimized 6% CoO x @C/g-C 3 N 4 composite exhibits superior catalytic efficiency and excellent cycling stability towards the degradation of various organic pollutants, which displays nearly 100% elimination of tetracycline (TC) within 80 mins. The h + , SO 4 •- and •OH are determined as the main contributors in the visible light-assisted PMS activation system, and the possible catalytic mechanism is also proposed. This work demonstrates a feasible strategy for constructing synergetic and effective photo-activation PMS catalysts for water remediation.
研究领域:
环境科学
·
化学工程
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材料科学
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 13
·10744-10752
·
IF 2.324
Liu Changhai,Wang Ke,Zhang Jin,Zheng Xuerui,Liang Qian,Chen Zhidong
Developing low-cost, efficient, and bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is an attractive yet challenging task. Herein, we report a novel, simple and one-pot method to fabricate ultrafinely dispersed Co-CoO x nanoparticles encapsulated in a nitrogen doped carbon nanotubes (denoted as Co-CoO x /CN) via an efficient thermal condensation of d -glucosamine hydrochloride, melamine and Co(NO 3 ) 2 ·H 2 O. A well-designed Co-CoO x based hybrid that possesses high activity and excellent durability for the OER and HER in alkaline solution has been fabricated. The catalyst displays good stability for 30,000 s and small Tafel slope of 82 mV per decade for OER and 110 mV per decade for HER. Detailed electrochemical and physical studies indicate that the high OER and HER activity of the hybrid catalyst arises from the strong interaction between Co-based NPs and N-doped carbon nanotubes, and especially the synergistic effect of Co and cobalt oxide.
研究领域:
材料科学
·
电化学
·
纳米技术
·
能量转换
·
催化
✓ 已验证
DOI
高影响因子
Environmental Science-Nano
·
2019
·Vol. 7
·期 2
·554-570
·
IF 7.704
Xinrui You,Chunyu Huang,Wei Huang,Guoyue Shi,Jingjing Deng,Tianshu Zhou
In this work, we have developed a novel method for preparing a CoOx/GO catalyst supported on ITO glass by electrochemical post-treatment of redox-active infinite coordination polymer (ICP) {Co(3,5-dbsq)(3,5-dbcat)(bix)} nanoparticles. Firstly, highly dispersed CoOx nanoparticles with ultra-small size and narrow size distribution (1.42 ± 0.34 nm) were in situ synthesized on ITO glass after electrochemical polarization of ICP coated on ITO glass at −1.1 V for 16.7 min (1000 s) in 0.10 mol L−1 KCl. Graphene oxide (GO) was next mixed with the ICP to obtain the CoOx/GO catalyst supported on ITO glass (the size of CoOx nanoparticles ranged within 1.21 ± 0.28 nm), which proved to have improved catalytic performance and enhanced stability compared to the pure CoOx. The catalytic activity of this CoOx/GO catalyst was then optimized according to the degradation efficiency of methylene blue (MB) via an advanced oxidation process in the presence of peroxymonosulfate (PMS). Under the optimal conditions here, the enhanced catalytic oxidative degradation of dye solution could be achieved easily. 100% of MB (2.0 mL, 20 mg L−1) could be decomposed within 6.7 min, which is better than other CoOx catalysts. With this kind of ITO glass as a component part, a portable reactor was constructed for the first time. Real-time monitoring of the catalytic degradation of colored wastewater from the textile and cosmetic industries was then achieved using this reactor directly by incorporating a UV/vis spectrometer, which is of great importance for information analysis and process control optimization during industrial wastewater treatment.
研究领域:
环境科学
·
催化
·
材料科学
·
化学工程
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Shufang Chang,Li Shi,Jinxing Yu,Ran Wang,Xiaoxiang Xu,Gang Liu
We have identified a facet-assisted mechanism for photocarrier separation in flux-treated Bi 4 TaO 8 Cl crystals that expose mainly {001} and {110} facets. These two crystal facets have different energy states that provide an internal electric field to split photocarriers towards different crystal facets. We have further leveraged the phenomenon by facet-selective deposition of CoO x cocatalyst at {001} crystal facets where holes are accumulated to expedite interfacial charge transfer reactions. The coupling of these two facet-engineering techniques brings exquisite control over the flow of photocarriers which cascade continuously from bulk to the surface for catalytic reactions . Under optimal conditions, the CoO x -deposited Bi 4 TaO 8 Cl achieves an unprecedentedly high apparent quantum efficiency of 27% at 420 ± 20 nm for water oxidation into O 2 . Stable overall water splitting into H 2 and O 2 (molar ratio 2:1) under visible light irradiation has also been realized in a Z-scheme system employing the CoO x -deposited Bi 4 TaO 8 Cl as the O 2 -evolution moiety.
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
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Xing Yang,Yunrui Tian,Shatila Sarwar,Miaomiao Zhang,Huaiping Zhang,Jujie Luo,Xinyu Zhang
Two nanocompisitees with different morphologies of polypyrrole nanofibers/cobalt oxide (PPyNF/CoO x ) and polypyrrole nanotubes/cobalt oxide (PPyNT/CoO x ) were successfully prepared via a rapid and cost-efficient microwave approach. The micromorphology, surface chemical and crystalline structure of the resultant samples were characterized by FT-IR, XRD , SEM and XPS . Besides, electrochemical performances of the as-produced nanocompisitees with different mass ratio, microwave powers and times were further investigated as a battery-type electrode materials for supercapacitors . It was found that the maximum capacitance of PPyNF/CoO x could reached up to 270C g −1 at 1 A g −1 , as well as with good cycling stability (almost nothing capacitance loss after 1000 cycles). Compared to PPyNF/CoO x , PPyNT/CoO x , showed a lower specific capacitance of 167.5C g −1 at the same current density. Surprisingly, the specific capacitance of PPyNT/CoO x could be further increased by 166% (278.4C g −1 at 1 A g −1 ) after 1200 cycles, and the cycling stability with nearly 105% of the initial capacitance could be achieved after 4000 cycles. Moreover, the asymmetric supercapacitor device based on the PPyNF/CoO x //active carbon showed a maximum gravimetric energy density of 24.22 Wh kg −1 and power density of 6.8 kW kg −1 , testifying its enormous potential for energy storage devices.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JACS Au
·
2021
·
IF 0
Maoyu Wang,Qingbo Wa,Xiaowan Bai,Zuyun He,Widitha S. Samarakoon,Qing Ma,Yingge Du,Yan Chen,Hua Zhou,Yuanyue Liu,Xinwei Wang,Zhenxing Feng
Restructuring is an important yet less understood phenomenon in the catalysis community. Recent studies have shown that a group of transition metal sulfide catalysts can completely or partially restructure during electrochemical reactions which then exhibit high activity even better than the best commercial standards. However, such restructuring processes and the final structures of the new catalysts are elusive, mainly due to the difficulty from the reaction-induced changes that cannot be captured by ex situ characterizations. To establish the true structure–property relationship in these in situ generated catalysts, we use multimodel operando characterizations including Raman spectroscopy, X-ray absorption spectroscopy, and X-ray reflectivity to investigate the restructuring of a representative catalyst, Co9S8, that shows better activity compared to the commercial standard RuO2 during the oxygen evolution reaction (OER), a key half reaction in water-splitting for hydrogen generation. We find that Co9S8 ultimately converts to oxide cluster (CoOx) containing six oxygen coordinated Co octahedra as the basic unit which is the true catalytic center to promote high OER activity. The density functional theory calculations verify the in situ generated CoOx consisting of edge-sharing CoO6 octahedral clusters as the actual active sites. Our results also provide insights to design other transition-metal-based materials as efficient electrocatalysts that experience a similar restructuring in OER.
研究领域:
电催化
·
材料科学
·
能量转换
·
原位表征
·
计算化学
✓ 已验证
DOI
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Yongjia Liang,Jianliang Zuo,Zhaohao Cai,Weican Huang,Jing Lin,Zili Liu
The ability to effectively control furan ring opening is the key to transforming furfural into 1,5-pentanediol. Herein, a series of Co-based catalysts modified with rare-earth metals (Y, Pr, La, and Ce) were synthesized. It was found that Y-modified Co-based catalyst with a Co/Y molar ratio of 3.5/0.5 exhibited the highest selectivity for 1,5-pentanediol (53.7%) at 150 °C and 4 MPa H2 in isopropanol (time = 5 h). Coordination between Co and Y in the catalyst resulted in more CoOx and oxygen vacancies, which are vital factors for cleaving the C–O bond of the furan ring. In addition, highly dispersed small-sized Co0 particles on the catalyst surface could boost the dissociation of H2 molecules, which attacked the carbonyl group in the furan ring of furfural to afford 1,5-pentanediol. Density functional theory calculations revealed that the presence of CoOx/Y2O3 oxide interfaces promoted adsorption of furfural (especially via the furan ring) and hydrogenolysis during the hydrogenation process. Modifying a Co-based catalyst with rare-earth metals offers a novel approach for producing 1,5-pentanediol from furfural.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 23
·8086-8093
·
IF 5.721
Haoxi Jiang,Debin Kong,Ying Niu,Sheng Wang
MnO2–CoOX catalysts with different Mn/Co ratios were prepared using polyvinyl pyrrolidone (PVP) as an assistant to control the morphology and exposed crystal faces of composite oxides. The physicochemical properties of the catalysts were systematically characterized and the catalytic activity of NH3-SCR and resistance to SO2/H2O were investigated. It was found that the NO conversion over Mn–Co-0.2-PVP was apparently higher compared with that over Mn–Co-X-PVP (X = 0.9, 0.8, 0.6, and 0.4). This can be interpreted in terms of exposed crystal surface (110) and enhanced adsorption of NH3/NO, and better redox performance resulting from higher Co3+/Co2+ ratio. Furthermore, different PVP and HAc additives have different H2O and SO2 resistance. Mn–Co-0.2-PVP showed good resistance to H2O and SO2 poisoning owing to having more low-temperature (∼200 °C) NO adsorption sites, which are beneficial to promote the de-NOX reaction and less affected by SO2.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Zong-Pin Fu,Qi-Jie Zhou,Yun-Peng Zhao,Yu-Fa Wu,Fang-Jing Liu,Mei Zhong,Jian Li,Jing Liang,Jing-Pei Cao
The high oxygen content and low calorific value of bio-oil make it unsuitable for direct production of high energy density fuels. To address this issue, the C-O-C, C-O-H, and C-C bonds in the oxygenated compounds of bio-oil can be modified through hydrodeoxygenation (HDO) reaction. In this study, we synthesized a series of efficient Ni-CoOx/Hβ-u catalysts by impregnating Hβ molecular sieve modified with urea under mild conditions. The catalytic HDO performance of these catalysts was evaluated using guaiacol and dealkalized lignin oil as substrates. The results indicate that the Ni-15CoOx/Hβ-u catalyst demonstrated superior activity. The suitable specific surface area and pore volume of the Ni-15CoOx/Hβ-u catalysts, as well as uniformly dispersed metal particles on their surface, increased the number of active sites available for HDO. Additionally, the presence of defective sites on the CoOx surface and acidic sites on the catalyst facilitate the breaking of intermediate C-O bonds (deoxygenation) and dehydration reactions. Utilizing the Ni-15CoOx/Hβ-u catalysts, guaiacol was completely converted to cyclohexane with 100% selectivity (at 180 °C, 1.0 MPa H 2 , 40 min). Furthermore, the phenolic compounds in bio-oil could also be transformed into cycloalkanes via the HDO process. These findings suggest that the Ni-15CoOx/Hβ-u catalyst has the potential to effectively hydrodeoxygenate bio-oil under mild reaction conditions.
研究领域:
能源化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）