JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2016
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IF 3.958
Mengshuai Liu,Bo Liu,Lin Liang,Fangxiao Wang,Lei Shi,Jianmin Sun
The novel bifunctional Zn/SBA-15 supported ammonium salt (NH 3 I-Zn/SBA-15) as single-component heterogeneous catalyst for the coupling of CO 2 with epoxides was developed. FT-IR, XRD, N 2 adsorption/desorption, TEM, XPS techniques were used to determine the morphological structure and physicochemical properties of NH 3 I-Zn/SBA-15 sample. The catalyst exhibited exceptionally effective activity with 93% yield and 99% selectivity and a high TOF of 306 h −1 to propylene carbonate at 130 °C and 3 MPa of CO 2 for 12 h in the absence of cocatalyst and solvent participation. Also the catalytic system was versatile to the cycloadditions of other epoxides with CO 2 under the optimized reaction conditions. Additionally, the catalyst was easily recycled and reused only with slight loss of activity after five recycles. Besides, a possible catalytic mechanism involving cooperative activation of epoxide and ring-opening by one-component and bifunctional catalyst was proposed. The protocol herein provides important insights on design of novel single-component heterogeneous catalysts for CO 2 relevant transformations.
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Advanced Healthcare Materials
·
2025
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IF 9.6
Jin Wu,Tao Meng,Xiaoqian Zhang,Songtao Tang,Lei Liu,Jing Xue,Xiaohui Liu,Junjun Wang,Jiyue Wen,Danyou Hu,Guiyang Zhang
Effective glycemic control is paramount for optimal wound healing in diabetic patients. Traditional antibacterial and anti-inflammatory treatments, while important, often fall short in addressing the hyperglycemic conditions of diabetic wounds. Therefore, the development of novel therapeutic strategies for accelerating diabetic wound healing has garnered escalating attention. Covalent organic frameworks (COFs) are an emerging class of crystalline porous polymers constructed through strong covalent bonds. Their exceptional structural tunability renders them as an ideal platform for advanced therapeutic applications. Herein, two redox-responsive Zn(II)-coordinated porphyrin COF hydrogels are constructed, which demonstrate rapid blood glucose reduction in localized tissues, along with improved angiogenesis, reactive oxygen species (ROS) scavenging, and photothermal antimicrobial capacities within the hyperglycemic blood environment of diabetic patients, thereby effectively controlling infections and concurrently promoting wound healing. Specifically, COFs with built-in dual active sites, i.e., disulfide or diselenide moieties, can be cleaved by ROS, releasing Zn(II) ions that possess antibacterial and tissue-repairing properties. Furthermore, the Zn(II)-porphyrin COF exhibits glucose oxidase (GOX)-like activity, catalyzing the conversion of glucose into non-glucose metabolites. This synergistic combination of glucose-responsive Zn(II) release and GOX-like activities effectively restores tissue redox balance and improves the wound microenvironment, offering a promising strategy for the diagnosis and treatment of diabetic wounds.
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DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Xiaohu Zhang,Guangyu Zhu,Fuyan Kang,Gege Zhang,Qianyun Tan,Min Wu,Yong Tan,Fa-Qian Liu
Herein, two-dimensional Zn(Bim)(OAc) nanosheets (ZNS) were prepared using ultrasonication and surfactant-assisted methods. Subsequently, it was used as nanocontainer loaded with benzotriazole (BTA) corrosion inhibitor to fabricate BTA@ZNS nanocomposites with pH-controlled release characteristics. The morphology analysis exhibits that BTA@ZNS has a distinct lamellar structure. UV spectrophotometer measurements indicated the release rate of BTA reached 94.38 % in 24 h at pH=1. Adding BTA@ZNS as fillers into epoxy resin (EP) coating can form BTA@ZNS/EP composite coating with active anti-corrosion properties. Electrochemical impedance spectroscopy (EIS) demonstrates that BTA@ZNS/EP coating has superior corrosion resistance than other EP-based coatings. The enhanced anti-corrosion performance is ascribed to the barrier effect and acid-responsive controlled release of BTA@ZNS.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Siyuan Sun,Fan Yang,Xiaoyun Zhang,Jinxiu Qian,Kexin Wei,Junpu An,Yang Sun,Shuyang Wang,Xi Li,Yongfeng Li
Transition metal single-atom catalysts (SACs) have been widely used in oxygen reduction reactions (ORR) and oxygen evolution reaction (OER) due to its greatest atomic utilization and low costs, which catalytic performance can be further enhanced by electron distribution adjustment. Herein, we synthesized a carbon-encapsulated FeS/Fe 3 C nanoparticles doped carbon-based Fe single atom catalyst from fluid catalytic cracking (FCC) slurry though a one-pot pyrolysis. The synergistic effect between FeS/Fe 3 C nanoparticles and Fe single atom structure (FeN x ) promotes the ORR/OER processes, which may due to the reduction of the adsorption free energy of intermediates. Meanwhile, the polyaromatic hydrocarbon in FCC slurry enhances the graphitization of catalyst to facilitate charge transfer in electrocatalysis process, and the carbon-encapsulated nanoparticles sites possess higher stability and dispersion. As a result, the optimized catalyst (FeS/Fe 3 C@Fe-N-C) presents a high nanoparticles dispersion and graphitization level, which has a higher ORR catalytic ability (E 1/2 = 0.91 V vs RHE) compared with commercial Pt/C (20 wt%, E 1/2 = 0.879 V vs RHE) and a similar OER catalytic ability (E 10 = 0.1.506 V vs RHE) compared with RuO 2 (E 10 = 1.518 V vs RHE). A liquid Zn-air battery assembled with FeS/Fe 3 C@Fe-N-C show a peak power density of 113 mW cm −2 and an open potential of 1.432 V. This work sheds light on a new method to design transition metal active sites carbon based single-atom catalyst for enhanced ORR and OER processes.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Haichuan He,Xiao Yu,Wei Wang,Liu Deng,Hao Zeng,Liqiang Wang,Ke Zeng,Jianhan Huang,Minghui Yang,You-Nian Liu
Bismuth-based materials have emerged as promising electrocatalysts for the electrochemical reduction of carbon dioxide (eCO 2 RR) to HCOOH. However, it remains challenges to meet the practical application requirements and identify the active sites of bismuth-based catalysts in eCO 2 RR. Herein, bismuthate (MBi 2 O 4 , M = Ca, Cu, Zn) derived nanosheet-like electrocatalysts with metal-modified edge defects are developed. During electrochemical processes, MBi 2 O 4 pre-catalyst undergoes surface reconstruction to expose more active Bi 0 sites and to form abundant metal-modified edge defects, which facilitate the modulation of charge state of adjacent Bi sites and improve the adsorption of *OCHO intermediate, thereby enhancing the selectivity of eCO 2 RR towards HCOOH. The Ca-modified defect-rich Bi catalyst exhibits a maximum HCOOH Faradaic efficiency of 94.3 % at an industrially relevant current density of 400 mA cm −2 , together with high stability/reproducibility of 55 h. This work proposes a new strategy for construction of Bi-based catalysts and explores its structural reconstruction mechanism during the electrocatalytic process, opening a new window for design of eCO 2 RR catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Xinmeng Yu,Xiaorong Chen,Dandan Yue,Fenghua Zheng,Qingyu Li,Zhaoling Ma,Hongqiang Wang
Aiming to achieve high-efficiency bifunctional catalysts, doping engineering is applied to construct bifunctional catalysts for oxygen electrodes in Zn-air batteries to strengthen the catalytic kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, MnS doped cobalt nitride catalyst (MnS/CoN x ) with divergent fiber morphology is prepared by low temperature nitriding for the self-assembling layered double hydroxides (LDH). The MnS/CoN x shows excellent electrical conductivity and improved catalytic activity on ORR and OER with low overpotential of 290 mV at 10 mA cm −2 and a good half-wave potential of 0.80 V in ORR compared with CoNx and MnO/CoN x . The contribution of the increased bifunctional catalytic performance is possible from the more active center Co 3+ and Mn 4+ , and the elevated electron transport resulted from the opportune high conductive MnS doping. The MnS/CoN x catalyst-driven Zn-air battery achieves a higher power density of 228 mW cm −2 and the excellent long-term stability of 500 h at 20 mA cm −2 far surpassing the commercial Pt/C+RuO 2 catalyst.
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Journal of CO2 Utilization
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2024
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IF 7.2
Qin Wang,Yuanping Zhang,Xiaoyun Li,Qian Chen,Maoqing Kang,Qifeng Li,Junwei Wang
The Zn–Co double metal cyanide (DMC) complex is regarded as a promising catalyst for the copolymerization of CO 2 and propylene epoxide (PO). Various methods have been adopted to improve the catalytic performance of DMC. In this study, polyvinylpyrrolidone (PVP), as a co-complexing agent, was innovatively used to modify DMC and applied to the synthesis of poly(ether–carbonate) polyols from CO 2 , PO, and a chain transfer agent. The modified catalysts exhibited higher catalytic activity than the catalysts prepared by conventional methods, with a nearly 10 % increase in PO conversion. The most critical breakthrough was a reduction of nearly 5 wt% in the byproduct propylene–carbonate. The results confirmed that amide groups in PVP could coordinate with active center Zn 2+ , providing the modified catalysts with advantages such as low-symmetry structure, high specific surface area, and strong acidity. Moreover, the dual effects of PVP coordination and dispersion led to dramatic differences in the microstructure and activity of the catalysts when added during different preparation processes of DMC. The coordination effect of PVP was dominant in the nucleation stages which affected the crystal structure and morphology, whereas, the dispersion effect was dominant in the aging stages which prevented the catalyst particles from growing and thus a higher specific surface area. This is critical for paving the way towards exploring the introduction of groups with high steric hindrance into Zn–Co complex catalysts. In addition, a detailed and in-depth insight into the structure–activity relationship of DMC for poly(ether–carbonate) polyols synthesis was summarized.
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Nano Materials Science
·
2024
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IF 12.6
Dezhi Jiao,Chengbao Liu,Yujie Qiang,Shuoqi Li,Cong Sun,Peimin Hou,Lanyue Cui,Rong-Chang Zeng
Coating microdefects and localized corrosion in coating/metal system are inevitable, accelerating the degradation of metal infrastructure. Early evaluating coating microdefects and detecting corrosion sites are urgent yet remain challenge to achieve. Herein, we propose a robust, universal and efficient fluorescence-based strategy for hierarchical warning of coating damage and metal corrosion by introducing the concepts of damage-induced fluorescence enhancement effect (DIE) and ionic-recognition induced quenching effect (RIQ). The coatings with dual-responsiveness for coating defect and steel corrosion are constructed by incorporating synthesized nanoprobes composed of metal organic frameworks (Ni–Zn-MOFs) loaded with Rhodamine B (RhB@MOFs). The initial damage to the coating causes an immediate intensification of fluorescence, while the specific ionic-recognition characteristic of RhB with Fe 3+ results in an evident fluorescence quenching, enabling the detection of coating damage and corrosion. Importantly, this nanoprobes are insensitive to the coating matrix and exhibit stable corrosion warning capability across various coating systems. Meanwhile, electrochemical investigations indicate that the impedance values of RM/EP maintain above 10 8 Ω cm 2 even after 60 days of immersion. Therefore, the incorporation of fluorescent nanoprobes greatly inhibits the intrusion of electrolytes into polymer and improves the corrosion protection performance of the coating. This powerful strategy towards dual-level damage warning provides insights for the development of long-term smart protective materials.
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ELECTROCHIMICA ACTA
·
2018
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IF 5.116
Hualin Lin,Daming Chen,Chenbao Lu,Chao Zhang,Feng Qiu,Sheng Han,Xiaodong Zhuang
The development of efficient and low cost electrocatalysts for oxygen reduction reaction (ORR) to replace precious metal-based catalysts is one of the emerging issues for wide applications of fuel cells and metal-air batteries . In order to develop better catalysts for ORR and study the effect of co-doping, in this work, we prepared S/N co-doped porous carbons by using commercially available monomers and the radical polymerization method. Besides, silica sphere hard template was also used to prepare porous carbons with hierarchical porous structure. Sulfur blending and ammonia activation were used to rational control the S/N ratios for the porous carbons. The as-prepared S/N doped porous carbons exhibit high specific areas up to 681 m 2 /g, high N and S contents up to 4.9% and 0.9%, respectively. As electrocatalysts in alkaline media, these porous carbons show high ORR activity with half wave potential up to 0.825 V vs . RHE, electron transfer number of 3.9 and good tolerance to methanol. As air cathode for Zn-air batteries, these porous carbons show peak power density of 10.7 mW cm −2 at 17.4 mA cm −2 . This work indicates that great potential of S/N -doped carbons as high efficient electrocatalysts for ORR and Zn-air batteries.
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JOURNAL OF SOLID STATE CHEMISTRY
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2018
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IF 2.179
Yong-Qiang Chen,Yuan Tian,Na Li,Sui-Jun Liu
Two isomorphous metal-organic frameworks (MOFs) {[M 2 ( μ 3 -OH)(trz)(sdba)(H 2 O)]·3H 2 O} ∞ (M = Ni for 1 , Zn for 2 , Htrz = 1,2,4-triazole, H 2 sdba = 4,4′-sulfonyldibenzoate) were obtained under the same reaction condition. Both of complexes present a three dimensional 8- c framework with whc1 topology based on M 4 -( μ 3 -OH) units. Moreover, the magnetic properties of 1 and anion sensing of 2 were investigated. The magnetic study show that the domain antiferromagnetic interactions exist in 1 . However, complex 2 can be considered as a promising chemical sensor for detecting PO 4 3¯ by means of fluorescence enhancement among various anions in aqueous solutions.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shuang Zheng,Lin Ding,Feilong Hu,Yong Zhang,Zhaofeng Ouyang,Shujuan Yang
In this work, the novel metal organic frameworks/multi-branched nanocellulose (Ni-Zn MOF@Multi CNC) fillers with different three-dimensional nanostructures are fabricated via two in-situ growing strategies, which were blended into Polyether sulfone (PES) matrix to construct composite ultrafiltration (UF) membranes. Furthermore, the effects of two structures of fillers on construction and performance of composite membranes are detailed investigated here. The results confirmed that the obtained PES composite membranes exhibited excellent permeability and selectivity because of the ultra-high hydrophilicity, abundant pores, and more negative charge of Ni-Zn MOF@Multi CNC fillers. Besides, compared with nanosphere structure of Ni-Zn MOF@Multi CNC, the nanoflower filler could provide more pores and cavities to enable higher water permeance, and more active surface charge (more -COO- groups) to increase protein rejection. The Ni-Zn MOF@Multi CNC 0.05 /PES membrane showed an 83 % higher permeance (up to 1151.00 L/m 2 h) and greatly improved BSA rejection (99 %). The Ni-Zn MOF@Multi CNC 0.05 /PES membrane has been successfully applied to different wastewater treatment, and shows expectant ultrafiltration performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yang Song,Caiyun Li,Jin Wang,Hongrui Yang,Hanwen He,Yukun Liu,Sen Zhang,Chao Deng
The explorations of efficient electrocatalysts to accelerate oxygen reactions in a wide temperature range is a crucial issue to the development of zinc-air batteries (ZAB) for all-climate applications. Herein, the Co-CoSe heterogeneous furry fibers (Co-CoSe@NHF) are developed as a bifunctional oxygen electrocatalyst for ZAB towards wide-temperature range applications. The Co-CoSe heterostructure with large work function difference (ΔW F ) endows interfacial electron redistribution, which builds strong interfacial built-in electric field (BIEF) and improves the oxygen reactions. Meanwhile, the Co-CoSe heterostructure is encapsulated by in-situ grown carbon nanotubes, and forms the hollow fiber (NHF) with furry surface and beads-on-string configuration. The highly porous and conductive NHF configuration facilitates the fast kinetics and favors to accommodates volume change during cycling. As a result, the Co-CoSe@NHF achieves the superior bifunctional properties and good reliability for oxygen reactions. Integrated with the Co-CoSe@NHF fiber, the ZAB cell delivers the superior power density (301 mW cm −2 ) and long-term cycling stability over 280 h at 25 °C, and maintains the power densities of 126 mW cm −2 even the temperature decreases to −25 °C. Moreover, the solid-state ZAB exhibits significant flexibility and superior properties in a wide temperature range. Therefore, this work not only proposes a new strategy to design the high-performance bifunctional electrocatalysts, but also propels the development of flexible power sources for all-climate applications.
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