Chem Catalysis
·
2024
·
IF 11.5
Bihua Hu,Bingxian Chu,Hailin Cao,Zhiwei Lei,Shuyu Cui,Peizhi Wang,Jun Tang,Xingzhu Wang,Baomin Xu
Molecular catalysts with precisely designed structures and abundant metal-nitrogen active sites have garnered significant attention for their ability to efficiently perform electroreduction of carbon dioxide (ERCD). However, the catalytic efficiency and selectivity are significantly limited by the fixed electronic structure of the metal-nitrogen structure, resulting in low production efficiency of more valuable products. This work presents the electronic regulation of cobalt phthalocyanine (CoPc) through in situ oxidation of N-doped Ti 3 C 2 T x nanosheets (CoPc/o–N–MXene). The resulting material exhibits high activity and tailorable selectivity. The study confirmed a strong interaction between Co-N 4 active sites and N–MXene after oxidation, resulting in a “Co–N–MXene” bond. This bond contributes to the transformation of intermediate ∗ CO into ∗ HCO, leading to a high selectivity of ERCD to methanol. This work provides a perspective on the mechanism of ERCD to methanol and an avenue for the synthesis of effective catalysts.
研究领域:
材料科学
·
催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yong-Sheng Li,Yi-Wei Gao,Yi-Kun Zhu,Heng Zhang,Wen-Shuang Zhang,Yong-Heng Yin,Yu-Xia Zhang,Chong-Bin Wang
Efficient Mg 2+ /Li + separation is highly demanded to address the global lithium scarcity. The nanofiltration (NF) membrane prepared with PEI-based monomer possess positively charged surface, exhibiting promise potential in lithium extraction from salt lake brines. In this work, water-soluble metal phthalocyanine (PEI@CoPc) was synthesized via grafting reaction between PEI and the (Tetracarboxyphthalocyaninato)cobalt(Ⅱ). The light-responsive NF membrane was prepared via interfacial polymerization technique using the water-soluble PEI@CoPc as aqueous phase monomer alone. This strategic modification significantly enhances the water permeance and Mg 2+ /Li + selectivity of the membrane. The best-performing of PEI@CoPc-TMC/PES membrane shows a water permeance of 16.7 L m -2 h −1 bar −1 and a Mg 2+ /Li + selectivity of 29.5. The membranes exhibited exceptional selectivity towards magnesium ions while maintaining high lithium permeability, offering effective technical support for the efficient extraction of lithium resources from salt-lake brines. Moreover, the distinctive photocatalytic activity of PEI@CoPc can generate active oxidizing species such as superoxide radicals (•O 2 – ) to oxidatively degrade pollutants, conferring the membrane excellent self-cleaning capability. The results indicated that the prepared composite membrane exhibit excellent fouling resistance and self-cleaning performance.
研究领域:
材料科学
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环境工程
·
化学工程
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高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 46
·17273-17278
·
IF 4
Li Zhang,Hong-Lin Zhu,Zhong-Yi Li,Yue-Qing Zheng
The exploitation of highly active and stable catalysts for reduction of CO2 and water oxidation is one of the approaches to facilitate scalable and sustainable CO2 reduction potentially at the industrial scale. Herein, a feasible strategy to rationally build an overall CO2 + H2O electrocatalytic reaction device is the preparation and matchup of a high-performance CO2 reduction catalyst and low-cost and highly active oxygen anode catalyst. A heterostructured nanosheet, γ-NiOOH/NiCO3/Ni(HCOO)2, exhibited superior catalytic activity in the oxygen evolution reaction, and was integrated with CoPc/Fe–N–C to build an overall CO2 + H2O cell with a current density of 10 mA cm−2 at a very low cell voltage of 1.97 V, and the faradaic deficiency of CO2 to CO was maintained at greater than 90% at 1.9 V.
研究领域:
能源化学
·
催化化学
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PubMed
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 10
·期 1
·2200738
·
IF 6.389
Bo Wu,Minzhang Li,Rajendran Ramachandran,Gaoqiang Niu,Mingxiang Zhang,Changhui Zhao,Zongxiang Xu,Fei Wang
Dopamine (DA) and uric acid (UA) are biomolecules of great consideration that coexist in human body. It is essential and challenging to detect them simultaneously with high sensitivity. This paper reports a novel electrochemical biosensor based on the nanocomposites of cobalt phthalocyanine (CoPc) anchored with graphene quantum dots (GQDs) for DA and UA detection. The GQDs incorporation on CoPc nanorods with partial end stretching significantly enhances the electrocatalytic activity and promotes the electron transfer rate. Low detection limits of 21 n m for DA and 145 n m for UA have been successfully achieved for the fabricated CoPc/GQDs biosensor. The density-functional theory proves the enhanced conductivity of CoPc/GQDs and the biomolecule's interaction with the electrode surface. Furthermore, the proposed sensor shows remarkable reproducibility, repeatability, and stability. The fabricated sensor is applied for the simultaneous detections of DA and UA in human urine samples. The excellent performance suggests that the CoPc/GQDs could be a promising and potential candidate for electrochemical sensors to detect DA and UA selectively.
研究领域:
生物传感器
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材料科学
·
分析化学
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高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Canyang Zhang,Guangtong Hai,Chao Chen,Yin Liang,Wei Zhao,Bolong Li,Jianghao Wang,Zhenyu Zhang,Huiping Ji,Kaige Wang,Reinout Meijboom,Jie Fu
The decarbonylation of biomass-derived fatty acids offers a green and sustainable route to high-value long-chain alkenes. Nitrogen-doped carbon-supported cobalt (Co-NC) catalysts have emerged as promising candidates for fatty acid decarbonylation, attributed to their exceptional catalytic activity and cost-effectiveness. However, identifying the active sites and elucidating the reaction mechanism remain significant challenges. To address these issues, we developed Co single-atom-rich catalysts (CoPc/MWCNT and pyrolyzed derivatives CoPc/MWCNT-X) via the impregnation of cobalt phthalocyanine onto multiwalled carbon nanotubes (MWCNTs), followed by pyrolysis. These catalysts exhibited a high stearic acid decarbonylation activity, increasing the heptadecene yield from 12.9 to 47.4%, with an alkene-to-alkane ratio of up to 4.3. Comprehensive characterization and control experiments conclusively demonstrated that Co single-atom sites serve as the active sites, while coexisting Co/CoO nanoparticles showed negligible activity and no synergistic effects. In situ DRIFTS revealed carbonyl group adsorption on Co single atoms, with DFT calculations confirming directional alkene production via C–O bond cleavage. This work establishes a facile synthetic strategy for high-performance decarbonylation catalysts and unambiguously identifies the critical single-atom active sites while enabling a profound understanding of fatty acid conversion mechanisms.
研究领域:
催化
·
绿色化学
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材料科学
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化学反应工程
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表面化学
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高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2019
·
IF 2.781
Qiang Liu,Lei Gao,Xingsong Su,Fei Zhou,Guotao Duan
The cobalt phthalocyanine (CoPc) resistance-type sensors to NO 2 were prepared using CoPc thin films via interfacial self-assembly method. Their sensing performances were investigated with respect to different NO 2 concentrations from 1 to 50 ppm. It was found that the CoPc sensors show excellent sensing performance: relatively low temperature (115 °C), high sensitivity (2.7–10 ppm NO 2 with a detection limit of 1 ppm), fast response and recovery (response time ∼26 s and recovery time ∼34 s at 3 ppm of NO 2 ), and excellent stability (almost the same after 4 weeks), reliability and selectivity towards NO 2 . Further, the sensitivity showed a quasi-linear relationship versus the concentration of NO 2 in the ranges of 1–50 ppm. On account of their high performances, the prepared CoPc thin films via interfacial self-assembly method will provide a high-efficiency sensor for practical NO 2 sensing applications.
研究领域:
材料科学
·
传感器技术
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INORGANIC CHEMISTRY
·
2026
·Vol. 65
·期 29
·16879-16886
·
IF 4.6
Wu Jing,Wang Ruonan,Lin Haifeng,Xing Jun,Wang Lei,Xu Jixiang
In this work, a novel ternary heterojunction consisting
of Zn vacancy-rich
zinc oxide (Zn 1– x O), a zeolitic
imidazolate framework-8 (ZIF-8), and cobalt phthalocyanine (CoPc)
was fabricated for photocatalytic N 2 fixation. The Zn 1– x O/ZIF-8 composite with bridged O–Zn–N
bonding was synthesized via in situ growth of ZIF-8 on Zn 1– x O, and it possessed a large surface area favorable
for N 2 adsorption. The incorporation of CoPc with dispersed
Co–N 4 (II) sites enhanced light harvesting and N 2 activation. Zn vacancies and coupled type II/Z-scheme charge
transfer pathways in the heterojunction accelerated the separation
of photogenerated charge carriers. As a result, the optimized catalyst
exhibited superior and stable photocatalytic N 2 reduction
performance via an alternating pathway in water, with an NH 4 + production rate of 65.2 μmol g –1 h –1 , which is 17.0 times higher than that of ZnO.
This study develops a novel ZnO-based heterojunction that simultaneously
optimizes multiple key factors for efficient photocatalytic N 2 fixation.
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ENERGY & FUELS
·
2026
·
IF 6
Tianxiang Guo,Baijiang Liu,Gujie Yao,Xiaoqing Wang,Yanyan Feng,Da Jin,Xilai Wang,Yarong Du
The electrochemical reduction of CO2 to high-value C2 products, especially ethanol, presents a feasible approach for alleviating greenhouse gas emissions and tackling climate-related challenges. Nevertheless, the rational design of efficient electrocatalysts is still restricted by insufficient activity, suboptimal selectivity, and a limited understanding of the underlying mechanisms. In this study, a hierarchically structured Cu-CoPc/CNT catalyst was fabricated by electrochemical deposition and drop-casting techniques. Comprehensive characterization (BET/SEM/XRD/EDS/XPS) confirmed its electronic configuration and surface properties. Electrochemical evaluations (CV/LSV/EIS/GC/1H NMR) demonstrated an ethanol Faradaic efficiency of 42.3% at a partial current density of 10.65 mA·cm–2, with exceptional ethanol selectivity of 98.6% among C2 products at −1.15 V vs RHE. In conjunction with density functional theory (DFT) calculations, mechanistic investigations have demonstrated that an adequate supply of those intermediates such *COOH and the facilitation of the C–C coupling are the primary factors contributing to the performance improvement of the CO2RR toward ethanol through the synergistic effect between CoPc/CNT and Cu. This research proposes a novel strategy for designing efficient and stable CO2-to-ethanol catalysts, thereby deepening the fundamental understanding of the ethanol formation mechanisms.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shihan Wang,Yuming Dong,Yongfa Zhu,Haifeng Shi
Polyethylene terephthalate is a major source of plastic pollution, posing significant environmental risks and requiring effective degradation methods. In the present work, the CuWO 4-x /Cobalt Phthalocyanine (CoPc) step-scheme (S-scheme) heterojunction was used as a photothermal-assisted photocatalyst to facilitate the degradation of polyethylene terephthalate via peroxymonosulfate activation in a cooperative photocatalytic system. The CuWO 4-x /CoPc sample exhibited optimal polyethylene terephthalate removal efficiency under the illumination conditions, reaching 83 % after the addition of 3 mM peroxymonosulfate. The influence of peroxymonosulfate dosage, aquatic environment, pH, and coexisting anions on polyethylene terephthalate degradation was thoroughly investigated. The X-ray photoelectron spectroscopy (XPS) and radical quenching experiment findings implied that the CuWO 4-x /CoPc composite followed the S-scheme heterojunction charge transfer process. Owing to the formation of the S-scheme heterojunction, the electron and hole transport and separation efficiency in the CuWO 4-x /CoPc photocatalyst was significantly enhanced. Infrared thermography images further revealed that the temperature rise of the solution during the catalytic process resulted from the photothermal property of CoPc, thus enhancing the degradation efficiency of polyethylene terephthalate plastics. Additionally, CuWO 4-x /CoPc demonstrated remarkable reusability and consistency in cycling experiments. This research presents an effective strategy by developing a photothermal-assisted S-scheme heterojunction system for the degradation of waste microplastics in aqueous environments.
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ACS Sensors
·
2023
·
IF 8.9
Chen-Xi Bi,Kai-Qi Jin,Jing Yan,Yu Qin,Feng Hong,Wei-Hua Huang,Yan-Ling Liu
Vascular smooth muscle cells (SMCs) are circumferentially oriented perpendicular to the blood vessel and maintain the contractile phenotype in physiological conditions. They can sense the mechanical forces of blood vessels expanding and contracting and convert them into biochemical signals to regulate vascular homeostasis. However, the real-time monitoring of mechanically evoked biochemical response while maintaining SMC oriented growth remains an important challenge. Herein, we developed a stretchable electrochemical sensor by electrospinning aligned and elastic polyurethane (PU) nanofibers on the surface of PDMS film and further modification of conductive polymer PEDOT:PSS-LiTFSI-CoPc (PPLC) on the nanofibers (denoted as PPLC/PU/PDMS). The aligned nanofibers on the electrode surface could guide the oriented growth of SMCs and maintain the contractile phenotype, and the modification of PPLC endowed the electrode with good electrochemical sensing performance and stability under mechanical deformation. By culturing cells on the electrode surface, the oriented growth of SMCs and real-time monitoring of stretch-induced H2O2 release were achieved. On this basis, the changes of H2O2 level released by SMCs under the pathology (hypertension) and intervention of natural product resveratrol were quantitatively monitored, which will be helpful to further understand the occurrence and development of vascular-related diseases and the mechanisms of pharmaceutical intervention.
研究领域:
生物材料
·
组织工程
·
生物医学工程
·
细胞生物学
·
电化学
·
心血管研究
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高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Nan Li,Ying Wang,Chenren Wu,Wangyang Lu,Kemei Pei,Wenxing Chen
Enzymes have always been a source of inspiration for the design and improvement of catalysts. Many examples are occurring in heme/non-heme metalloenzymes with the generation of active high-valent metal-oxo intermediates that are controlled by the surrounding amino acids/protein and axial residue ligands, facilitating the efficient oxidation of substrates in biochemical processes. Here, the high-valent cobalt-oxo species have been formed during the heterolysis of H 2 O 2 activated by the bioinspired catalyst, axially coordinated cobalt phthalocyanine (CoPc) on pyridine-functionalized multi-walled carbon nanotubes (MWCNTs-Py), characterized by ultraviolet–visible and X-ray photoelectron spectroscopy. Formation process of the active cobalt-oxo species has been further confirmed by electrospray ionization mass spectrometry analysis and the results from the density functional theory (B3LYP/6-311G) calculations. Such high-valent cobalt-oxo species exhibit high reactivity and enough persistence for the oxidation of the target substrate, C.I. Acid Red 1. The oxidation products are nearly biodegradable small molecules identified by ultra-performance liquid chromatography/high-definition mass spectrometry. This strategy provides a foundation on developing efficient and persistent catalytic system, in particular oxidation processes based on the complex catalysts with N 4 macrocycle structures.
研究领域:
环境科学
·
催化化学
·
材料科学
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高影响因子