PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
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IF 7.926
Yan Shao,Han Wu,Wenshan Huang,Qijie Jin,Longji Wu,Xueying Zhang,Haitao Xu
For the treatment of antibiotics contained wastewater, developing a highly efficient catalyst is key to peroxymonosulfate (PMS) activation and antibiotics degradation. In this work, nitrogen-doped carbon nanosheets (NCS) coated sintered metal fibers (SMFs) catalyst was designed and developed, which could positively promote the contacting efficiency between PMS , TC and catalysts. In specific, by the dip-coating of SMFs in the cobalt-contained dicyandiamide formaldehyde resin and the following pyrolyzing coordinated polymer procedure, it was possible to create a Co-doped NCS catalyst supported on SMFs. NCS with abundant exposed surface active sites could result in a relatively higher catalytic activity . Microscopy studies confirmed the presence of stacked NCS with high Co active sites loading, which was anchored on the surface of SMFs. The developed Co NCS/SMFs catalyst exhibited a highly degradation efficiency of 96% in 240 min. Effects of operating parameters (including PMS concentration and solution pH) on the TC elimination efficicency were also investigated. Additionally, Co NCS/SMFs exhibited good PMS activation activity in the wide pH range of 2.0–9.0, and acceptable recyclability with over 86% TC removal efficiency after five cycles test. According to SEM , XRD and XPS results, highly exposed active metal sites, O defects, Co-N x sites and reactivity of Co 0 in Co NCS/SMFs played an important role in the enhancement of degradation efficiency. Finally, radical inhibition experiment and corresponding EPR test revealedthe presence of S O 4 ∙ − , ∙OH , O 2 ∙ − and 1 O 2 in the TC degradation system, in which singlet oxygen ( 1 O 2 ) was demonstrated to be the dominating reactive species for PMS activation and TC degradation. This work provided an efficient strategy for developing robust monolithic lamellar catalyst for the continuous PMS activated degradation of TC.
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Chemosensors
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2022
·Vol. 10
·期 11
·443
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IF 4.229
Luyi Zhu,Qinan Zhou,Wenqing Shao,Zhenbo Wei,Jun Wang
A novel Co-based organic frameworks/carbon nanotubes/silicon dioxide (Co-MOF/CNTs/SiO2)-modified Au electrode was fabricated and taken as a platform for gallic acid (GA) detection. The composite combined the advantages of Co-MOF, CNTs and SiO2, and higher electrochemical response of Co-MOF/CNTs/SiO2-modified electrode indicated that the composite material exhibited satisfied the catalytic activity towards GA. Moreover, the electrochemical oxidation process of GA was deeply investigated on the surface of electrode based on computational investigations. Hirshfeld charges and condensed Fukui functions of each atom in GA were calculated. Besides, the catalysis of Co-MOF to GA was further investigated based on density functional theory. The quantitative determination of GA was carried out and showed a linear range between 0.05–200 μM, with low limit of detection. The sensitivity value of the self-assembled electrochemical sensor was calculated to be 593.33 μA cm−2mM−1, and the selectivity, reproducibility and stability of the gallic acid sensor were also confirmed in the study.Keywords:gallic acid;electrochemical;electro-oxidation;detection;density functional theory
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Zhenyu Liu,Xiaoman Li,Senda Su,Wenming Ding,Linghu Meng,Yingying Wang,Mengyao Tan,Min Luo
Energy band engineering strategy by doping has been extensively proved to have great influence on photocatalytic properties of semiconductors. Herein, a novel Co-doped Bi 2 MoO 6 (Co-BMO) photocatalyst was developed for photocatalytic nitrogen fixation. Co-BMO with microsphere structure was synthesized by a one-step solvothermal method. The NH 3 yield of 0.3 % Co-BMO (130.07 μmol·h −1 ·g cat −1 ) was about 3.9 times higher than that of pure BMO without scavengers and visible light irradiation. The band gap of 0.3 % Co-BMO was reduced and the average PL lifetime was improved due to the successful doping of Co 2+ , which directly led to higher separation efficiency of photogenerated carriers and improved photocatalyst activity. In addition, gas chromatography (GC) tests showed that 0.3 % Co-BMO had a higher photocatalytic oxygen production capacity, which meant that more protons would be involved in the nitrogen reduction reaction . Their synergistic effect greatly enhanced the photocatalytic nitrogen fixation ability of 0.3 % Co-BMO. This novel photocatalyst may be a promising candidate for photocatalytic nitrogen fixation.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Wenyu Guo,Shuo Huang,Jian An,Jiabin Zhang,Feihong Dong,Jie Dang,Jue Zhang
As one of the most valuable endogenous gas signaling molecules, carbon monoxide (CO) has been demonstrated in numerous studies to show excellent promise in the treatment of diseases, such as cancer. However, for many years, the inherent high affinity of CO for hemoglobin severely impeded the clinical transformation of CO-based treatments. Therefore, the controlled delivery of CO to target tissues has become a common challenge. Herein, an efficient ultrasonic-triggered and targeted CO release strategy was constructed based on a novel targeted acoustic release carrier of carbon monoxide (TARC-CO) that we synthesized in this study. The designed TARC-COs could afford a safe, stable, and ultrasound-guided delivery of CO in vivo by loading a specified dose of CO inside microbubbles, resulting in breast tumor suppression. Taking advantage of the high loading capacity of microbubbles, the unit volume of TARC-CO suspension could encapsulate up to 337.1 ± 8.0 (×103 ppm) of CO. In addition, the satisfactory ultrasound contrast-enhanced ability of TARC-COs achieved real-time interactive guidance and visual policing of CO delivery. For the in vitro antitumor study, TARC-COs with ultrasonic irradiation were demonstrated to effectively induce mitochondrial dysfunction by reducing mitochondrial membrane potential, leading to the apoptosis of 4T1 cells. In addition, we realized that TARC-CO-based treatment could significantly slow the growth rate of tumors by inducing apoptosis, inhibiting the proliferation of cancer cells, and limiting tumor angiogenesis. In summary, this proof-of-concept study demonstrates the feasibility and tremendous potential of TARC-COs for controlled release of CO, which can be expected to provide new inspirations and a promising perspective for therapy based on active gases.
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PubMed
高影响因子
ACS Omega
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2022
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IF 4.132
Tianxiang Jin,Jingwei Su,Qingyun Luo,Wei Zhu,Haizhen Lai,Dejuan Huang,Chunyan Wang
Biomass-derived activated carbon is a widely used electrode material for supercapacitors. One of the keys to preparing high-performance activated carbon is the selection of appropriate precursors. Daylily is a common edible herb and is widely planted in Asia. It is rich in nitrogen and phosphorus, so it can be used as a precursor of heteroatom-doped activated carbon. Herein, a daylily-derived porous carbon with a large specific surface area and high content of heteroatoms has been successfully prepared by a simple carbonization method. The as-prepared carbon materials showed a remarkable specific capacitance of 299.1 F/g at 0.5 A/g and excellent cycling stability of 99.6% after 4000 cycles at a current density of 1 A/g. Moreover, the assembled symmetric supercapacitor showed a high energy density of 21.6 Wh/kg at a power density of 598.2 W/kg in 6 M KOH electrolyte. These results demonstrate that the daylily-derived porous carbon is an excellent material for high-performance supercapacitors.
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PubMed
高影响因子
CARBON
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2022
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IF 11.307
Dandan Han,Qian Zhou,Yan Xia,Dongting Huang,Jieqiong Qin,Lixia Wang,Xiaopeng Wang,Xianfu Zheng,Dan Wu
The bottom-up assembly utilizing nanocrystals (NCs) as building blocks is a highly anticipated approach to access novel metamaterials. Limited by the library of binary spherical assembly, colloidal components of building blocks are necessarily extended for targeting the desired assembled-superstructure with emergent properties. Here, a generalized approach is presented that carbon nanotubes (CNTs) capped with long-chain hydrocarbon ligands, as creative colloidal components, can be compatibly co-assembled with various NCs into binary supraspheres based on a confinement microemulsion environment. Such cross-dimensional assemblies possess the structural merits of excellent conductivity, abundant voids and high stability, thus synergistically boosting its electrochemical performance. As a proof of concept , the co-assembled CoFe 2 O 4 /CNTs supraspheres exhibit extraordinary capacity (890 mAh g −1 at 0.5 A g −1 ), rate capability (318 mAh g −1 at 20 A g −1 ), and structural stability (458 mAh g −1 at 5 A g −1 after 1000 cycles) relative to pure CoFe 2 O 4 when evaluated in Li-ion battery. Beyond that, its derived phosphides CoFeP/CNTs assemblies outperform most of the state-of-art electrodes when acting as electrocatalysts for hydrogen evolution reactions (HER). This work provides a new perspective for constructing superstructures of NCs for potential applications in energy storage devices.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Lina Zhang,Yutao Jia,Han Hao,Mi Wang,Jing Wang
Mitochondria-targeted therapeutic strategies are widely used in the targeted delivery of anti-tumor drugs to achieve effective and precise treatment. Herein, a pH-responsive and mitochondria-targeted liposome-enveloped methoxylated covalent organic framework (mCOF) delivery system loaded with doxorubicin (DOX) and camptothecin (CPT) is constructed. Different from introducing additional mitochondria-targeting molecules, we incorporate amphiphilic DOX-lipid molecules into a lipid bilayer to achieve mitochondria-targeted and therapeutic agent delivery (DOX) to induce oxidative stress in tumor mitochondria. Furthermore, CPT, which can also induce mitochondrial oxidative stress, is co-loaded with DOX-lipid using mCOF with high porosity to enhance the synergistic therapeutic effects. In addition, cholesteryl hemisuccinate is assembled with amphiphilic DOX-lipid on the surface of the mCOF to achieve pH-sensitive drug release. Consequently, the DOX-CPT dual drug-loaded delivery system with mitochondria-targeted ability can efficiently increase the level of reactive oxygen species in the mitochondria and enhance anti-tumor efficacy compared with other groups. Given its good biocompatibility, the constructed dual drug delivery platform based on liposome-enveloped mCOF synergistically combines mitochondria-targeted DOX-lipid with mitochondria-acted CPT, which provides a feasible strategy for organelle-targeted combination chemotherapy to improve therapeutic effects.
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POLYMER DEGRADATION AND STABILITY
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2022
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IF 5.204
Congling Shi,Mei Wan,Zhengbo Hou,Xiaodong Qian,Honglei Che,Yueping Qin,Jingyun Jing,Jian Li,Fei Ren,Bin Yu,Ningning Hong
Thermoplastic polyurethane (TPU) is the most used polyurethane, but its highly flammable characteristic restricts its extensive use. In this work, Co-MOF@MXene hybrids flame retardants were synthesized and incorporated into TPU . The flame-retardant characteristics of TPU composites were investigated by cone calorimeter test and thermogravimetric analyzer. Compared with TPU, the peak heat release rate and total heat release rate of TPU/Co-MOF@MXene composites were reduced by 28.3% and 14.5%, respectively; and the smoke production rate and total smoke production of the composites with only 2 wt% Co-MOF@MXene hybrids were also reduced by 58.8% and 47.5%, respectively. Furthermore, the char residues of TPU/Co-MOF@MXene composites were about 2 times that of pure TPU. Systematical characterizations were then carried out to investigate the flame retardant mechanism of Co-MOF@MXene hybrids, highlighting the barrier effects of MXene combined with the catalytic effect of Ti and Co. The hybrids flame retardants greatly benefit the further development of TPU nanocomposites.
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MATERIALS LETTERS
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2022
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IF 3.574
K.P. Li,Z.Z. Liu,Y.Q. Zhang,X.B. Yang,B. Zhou,Z.X. Xie,Z.Q. Duan,Y.M. Hu
The most used counter electrodes (CEs) in dye-sensitized solar cells (DSCs) are made of platinum (Pt). However, the cost of Pt CEs is expensive. In addition, the poor corrosion resistance of Pt in liquid electrolytes hinders commercialization of DSCs. Sulfides are potential CE materials due to their excellent catalytic performance and low cost. Nanocrystalline Cu 2 Cu 1-x-y Fe x Mn y SnS 4 (CCFMTS) CEs were fabricated using Fe and Mn co-alloyed Cu 3 SnS 4 (CTS) by an easy process of a spin-coating coupled with a post annealing. Electrochemical and photovoltaic properties of the DSCs assembled with the CCFMTS CEs were analyzed by EIS, Tafel and J-V tests. Electrochemical results show that series resistance ( R s ) and charge transfer impedance ( R ct ) at the CE/electrolyte interface of the cells decreased by 21.68% compared with the cell with unalloyed CTS CE, while exchange current density ( J 0 ) and limiting diffusion current density ( J lim ) were increased, which indicates conductivity and electrocatalytic activity of the CEs were improved after the co-alloying. As a consequence, the maximum actual output power ( P max ) of the cells was enhanced. In the optimal case, photovoltaic conversion efficiency (PCE) of 7.16% was achieved which is 84.83% of that of the cell with Pt CE.
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Catalysis Science & Technology
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2022
·Vol. 12
·期 14
·4486-4497
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IF 6.177
Si Liu,Zhenfu Wang,Kun Chen,Linling Yu,Qinghong Shi,Xiaoyan Dong,Yan Sun
Chiral amines are valuable intermediates widely applied in the pharmaceutical industry. As an alternative to classical synthetic methods for the production of chiral amines, biocatalytic cascade synthesis for these molecules from their alcohol precursors has been developed. However, currently available enzyme cascade systems remain unstable and unsustainable in the practice of chiral amine synthesis. Herein, the catalytic cascade system of chimeric amine dehydrogenase (AmDH) and alcohol dehydrogenase (ADH) fused with silica binding peptide (SiBP) was site-specifically co-immobilized on silica nanoparticles (SNPs). SiBP enabled the fusion enzymes to firmly bind to SNPs, and both the single immobilized enzymes showed higher catalytic efficiencies (kcat/Km) than their free counterparts to different degrees. Using 10 mM (S)-2-hexanol as the substrate, the co-immobilized enzyme system (SiBP–ADH&SiBP–AmDH@SNPs) showed 90% (R)-2-aminohexane yield after 48 h reaction, which was 1.85-fold higher than the free enzyme system due to the enhanced catalytic efficiency of the immobilized enzymes and the possible proximity effect of the SiBP–ADH&SiBP–AmDH@SNPs. The catalyst productivity of the SiBP–ADH&SiBP–AmDH@SNPs was 11 to 34 times higher than literature data, demonstrating the high economic benefits and catalytic efficiency of this system in producing chiral amines. SiBP–ADH&SiBP–AmDH@SNPs retained 87% of its original activity after eight cycles of reuse. These results highlighted the potential of the co-immobilization system for the effective and sustainable synthesis of chiral amines in industrial practice.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Pan Li,Xinbao Li,Yang Wang,Pengfei Shen,Xinbo Zhu,Yingying Zhu,Zan Wu
A low-cost, high-performance catalyst for phenol steam reforming (PSR) at low temperature was prepared by introducing waste coal ash into Co/Al 2 O 3 . The optimized content of coal ash in the catalyst were ranged from 50 to 65 wt%, presenting over 97% phenol conversion and 92% H 2 yield at low temperature of 450 °C. The stability for the best catalyst with an ash content of 50 wt% exceeded 85 h. Two-step reduction of Co 3 O 4 to Co 0 via CoO was identified by in-situ XRD. DFT calculations showed that phenol adsorption and decomposition were preferred on the FeCo bimetal surface rather than the single Co surface. H 2 O adsorption and dissociation fascinated on the CaO incorporated Al 2 O 3 surface. Both Fe and Ca in the coal ash improved the catalyst performance in PSR at low temperature. This work gives an opportunity to solve the drawbacks of high reaction-temperature and low catalyst-stability in PSR, and furthermore benefits to get a deep insight into the reaction mechanism of PSR over the catalyst.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2022
·Vol. 46
·期 13
·18624-18633
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IF 4.672
Honghong Cheng,Bo Li,Tao Meng,Cong Liu,Dong Shu
Summary Practical applications of graphene-based materials are still inhibited by the serious restacking of graphene nanosheets and single electrical double-layer capacitor energy storage mechanism. To address these issues, nitrogen/sulfur-co-doped reduced graphene oxide (N/S-rGO) was ingeniously prepared by supermolecular-driven in-situ co-dope method. In this article, the GO/L-cysteine supermolecular system was assembled first, the hydrogen bond between L-cysteine and GO is confirmed by the Fourier-transform infrared spectroscopy (FTIR). The theoretical calculation result indicating that L-cysteine is uniformly assembled on GO surface by supermolecular interaction force (dispersion force and hydrogen bond). Due to the oriented supermolecular force, the thus-fabricated N/S-rGO affords customized three-dimensional (3D) porous structure, uniform N,S co-doping, effective electrolyte ion-transport pathways, and satisfactory structural stability. Attributing to the inherent plentiful 3D cavity structure and synergistic effect between N, S heteroatoms, N/S-rGO shows outstanding electrochemical performance, the best-performed N/S-rGO2 possess delightful capacitance (416 F g −1 ), after 20 000 cycles the capacitance retention of N/S-rGO is 110% of the initial value, shows excellent cycle reliability. The N,S-rGO all-solid flexible symmetrical supercapacitor can light up luminous diode for 30 seconds when fully charged, indicating that it provides the possibility of practical application.
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