ELECTROCHIMICA ACTA
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2022
·
IF 7.336
Jie Li,Youcai Lu,Shiyu Ma,Zhongjun Li,Qingchao Liu
Li–O 2 battery has attracted wide attention because it can satisfy the need for a new energy storage system with high energy density. However, poor oxygen reduction (ORR)/oxygen evolution (OER) kinetics involving Li 2 O 2 formation/decomposition is a major obstacle to its development. By designing suitable cathode with desired structure and surface electronic states, the formation/morphology of Li 2 O 2 and the reaction kinetics of charge process can be efficiently optimized simultaneously. In this work, a novel sulfur (S) and chlorine (Cl) co-doped porous carbon (CSC) were synthesized by one-step pyrolysis strategy, and the amount of heterogeneous atoms could be flexibly controlled by different calcination temperatures . Experimental combined with theoretical calculations show that the content of C Cl bond plays an important role in the adsorption of intermediate LiO 2 , thus regulating the morphology of Li 2 O 2 and ultimately affecting the release of battery energy. The C S bond mainly acts on the dynamics of the ORR and OER processes, which has an important influence on improving the round-trip efficiency of the battery. Benefiting from the synergistic effect of heteroatoms , the electrochemical performances of the Li–O 2 battery, including round-trip efficiency, discharge capacity and cycling stability are greatly improved.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Hao Wang,Yongrong Zou,Tao Luo,Mehdi Benouahmane,Danna Zhou,Feng Wu
In recent years, a new strategy of using sulfite (S(IV)) to replace persulfates (peroxydisulfate (PS) and peroxybisulfate (PMS)) for sulfate radical based advanced oxidation process (SR-AOP) has emerged as one of the potential alternatives in the field of AOPs. Although the thermal activation of PS and PMS has been investigated extensively, that of S(IV) has not yet been explored. In this work, As(III) oxidation in a heat–S(IV) system was investigated first to demonstrate the feasibility of thermal activation of S(IV). Results showed that S(IV) can be activated to oxidize As(III) by heating the reactant solution from room temperature to above 50℃. Almost complete oxidation of 5 μM As(III) in water at pH 7 with addition of 1 mM S(IV) was achieved at 70 °C within 30 min. As(III) oxidation in the heat–S(IV) system was strongly dependent on the dissolved oxygen in water. Radical-scavenging experiments and electron spin resonance analysis demonstrated that the main active species responsible for As(III) oxidation was SO 4 •− . On the basis of thermal activation, a new system of SR-AOPs, namely, heat–electro-S(IV) system, the coupling thermal and electrochemical activations was established with ruthenium-plated iridium electrodes at a voltage of 3 V. It achieved complete oxidation of 50 μM As(III) in water at pH 7 at 50 °C with the addition of 2 mM S(IV) after reaction for 30 min. This work provides a new activation method for SR-AOPs with S(IV) as the precursor of reactive species and helps in understanding the reaction of S(IV) autooxidation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jiangfu Zheng,Changzheng Fan,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Jinglin Ding,Shengxiang Rong,Zhuo Chen,Jun Luo,Baowei Zhang
A novel hexagonal AgBr/Zn-Al MMO S-scheme photocatalyst was prepared by adopting a simplified hydrothermal and co-precipitation method. The prepared photocatalytic system exhibited excellent photocatalytic performance in degradation of tetracycline hydrochloride (TC). In particular, the ABMO0.2/Vis system generated the best TC removal rate (95%) within 60 min of visible light irradiation. Moreover, no significant decrease of the photocatalytic performance had been observed after four cycles, while the leaching of silver ions was effectively controlled. The excellent photocatalytic performance can be attributed to the synergistic effect occurring between the unique morphological structure and the S-scheme heterojunction charge transfer mechanism, since that that synergistic effect enhanced light absorption capacity and separation efficiency of the photogenerated carriers and the redox ability. In addition, liquid chromatography-mass spectrometry (LC-MS) analysis clarified the mineralization behavior and detailed decomposition pathways of TC. This work opens a new pathway for the design of efficient S-scheme heterojunctions and provides new insights into the photocatalytic degradation mechanism of antibiotics.
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高影响因子
CARBON
·
2022
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IF 11.307
Meizhe Yu,Xiuzhi Guo,Haojie Lu,Peili Li,Ruobing Huang,Chunning Xu,Xuedong Gong,Yuhong Xiao,Xiaodong Xing
Developing efficient and safe approach to counteract the bacterial infections has become an urgent clinical challenge. In this work, we report folic acid derived carbon dots (FA-CDs) prepared by a one-step pyrolysis method. The FA-CDs can respond to the environmental stimuli of bacterial infections and acquire antimicrobial capacity “on demand” as a simple and effective antimicrobial nanosystem. The assays on antibacterial properties and mechanism show that FA-CDs are able to induce the gradual increase of intracellular reactive oxygen species (ROS) levels in bacteria under the simulated acidic environment and display pH-responsive biocidal activity. In a neutral condition, FA-CDs have no antibacterial activity, which will be conducive to mitigating the rise of bacterial drug resistance. The responsive antibacterial behavior can be attributed to that FA-CDs exhibit distinctive oxidase-like and peroxidase-like activity under acidic stimuli and inhibit the superoxide dismutase activity in bacteria cells, causing the accumulation of intracellular ROS. Meanwhile, FA-CDs can selectively kill Gram-positive bacterium S. aureus and remove mature biofilms. Besides, the in vitro and in vivo experiments demonstrate that FA-CDs possess excellent biocompatibility, and show remarkable therapeutic effect on the S. aureus -infected back wound models of mouse, which are crucial for clinical applications. Thus, this study highlights the potential application of FA-CDs as an ultra-succinct smart antimicrobial nanosystem for coping with infections caused by S. au reus in the clinical setting, and will bring about a new perspective on developing antimicrobial CDs.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yabin Li,Jingyao Qi,Jimin Shen,Pengwei Yan,Jing Kang,Binyuan Wang,Shuyu Wang,Jinxiang Zuo,Zhonglin Chen
Peroxymonosulfate (PMS)-based advanced oxidation processes are perceived as a novel strategy for water purification. However, designing an efficient catalyst with a low metal leaching rate remains challenging. Here, under palygorskite (PAL) mediation, 16%-CoCu 0.4 Fe 1.6 O 4 @PAL (16%-CCFO@PAL) was constructed, exhibiting ample oxygen vacancies (V O ) and low metal leakage. The V O was confirmed by systematic characterizations and theoretical calculations. The catalyst showed the efficient catalytic capacity for PMS by dual-path (i.e., metal sites and V O ) activation. Large amounts of SO 4 •- , •OH, and 1 O 2 were produced, greatly destroying bisphenol S (BPS). BPS removal was greater than 99% within 25 min in the 16%-CCFO@PAL/PMS system. At the metal sites, PMS was activated under the synergistic effects of Co(II)/Co(III), Fe(II)/Fe(III), and Cu(I)/Cu(II) pairs and electron transfer. In addition to metal sites, the V O was also an activation center for PMS, which mainly captured the O I atom in [H-O I -O II -SO 3 ] - , donating an electron to O I and promoting SO 4 •- generation. The interfacial reaction mechanism was explored by in situ tests, and a dual-path activation mechanism was proposed. This work provides a new perspective for V O -assisted PMS activation for water treatment.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Lina Wang,Yun Zhao,Lijuan Cao,Yong Li,Gaoyi Han,Canliang Ma,Zongping Shao
Exfoliated graphite (EG) as important matrix material for potassium-ion batteries (PIBs) suffers from its inherent low surface activity, which results in poor interactions with active matter (e.g. metal sulfides) and undesired initial capacity decay of the EG-based electrodes. To address these issues, in this study, an attempt for EG’ surface engineering has been carried out through a stepwise gas-phase strategy. A S-doped carbon nanofiber/nanotube (CNF/CNT) hybrid was in-situ introduced on the surface of EG to form a novel micro-/nano- multiscale matrix structure. CoS nanoparticles are encapsulated in the inner of CNFs and CNTs. The special core–shell configuration not only prevents the aggregation of CoS during the sulfidation process, but also confines the active nanoparticles to avoid pulverization and maintains stable integrated electrode structure. Moreover, the couple effect between the active site-rich nature of CNFs and the high conductivity of CNTs as well as the formation of 3D porous network contribute to substantially elevated reversible capacity (411 mAh g −1 ), excellent initial cycling stability and rate capability (184 mAh g −1 at 2.0 A g −1 ). The effective surface modification strategy dominated by rational hybridization of CNFs and CNTs provides a new avenue for the development of high-performance electrode materials in PIB applications.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Yingcong Wei,Qiqi Zhang,Ying Zhou,Xiongfeng Ma,Lele Wang,Yanjie Wang,Rongjian Sa,Jinlin Long,Xianzhi Fu,Rusheng Yuan
Simultaneous generation of H 2 fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy. Herein, for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol (BA) into benzaldehydes (BAD) and H 2 , a novel localized surface plasmon resonance (LSPR) enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO 3– x as oxidation semiconductor and Zn 0.1 Cd 0.9 S as reduction semiconductor. The photoredox system of Zn 0.1 Cd 0.9 S/MoO 3– x displayed an unconventional reaction model, in which the BA served as both electron donor and acceptor. The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically. Moreover, due to the LSPR effect of MoO 3− x nanosheets , Zn 0.1 Cd 0.9 S/MoO 3− x photocatalysts exhibited strong absorption in the region of full solar spectrum. Therefore, the Zn 0.1 Cd 0.9 S/MoO 3− x composite generated H 2 and BAD simultaneously via selective oxidation of BA with high production (34.38 and 33.83 mmol·g −1 for H 2 and BAD, respectively) upon full solar illumination. Even under NIR light irradiation, the H 2 production rate could up to 94.5 mmol·g −1 ·h −1 . In addition, the Zn 0.1 Cd 0.9 S/MoO 3– x composite displayed effective photocatalytic H 2 evolution rate up to 149.2 mmol·g −1 ·h −1 from water, which was approximate 6 times that of pure Zn 0.1 Cd 0.9 S. This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Zhengzheng Guo,Penggang Ren,Jin Wang,Xin Hou,Jiahui Tang,Zongbin Liu,Zhengyan Chen,Yanling Jin,Fang Ren
The development of absorption-dominant electromagnetic interference (EMI) shielding materials with high-efficiency EMI shielding effectiveness (SE) and low reflection (R) is crucial but challenging for next-generation electronics devices and telecommunication. In this regard, a facile and environmentally friendly approach was proposed to fabricate N, S- co -doped TiC/carbon hybrid aerogels with hierarchically porous architecture through MXene/cellulose hybrid hydrogels as precursors for adsorbing dyes, followed by freeze drying and carbonization process. Profiting from the synergistic effect of highly interconnected three-dimensional (3D) porous structure, heterogeneous conductive network with greatly conductive difference as well as heteroatoms-doping induced dipole polarization, the resultant aerogel with an ultra-low density (47.1 mg/cm 3 ) achieves a highly efficient EMI SE of 84.3 dB at 12.4 GHz (average 81.8 dB in the X-band) and a superior absorption coefficient of 0.68 simultaneously. Meanwhile, the highly porous structure endows the prepared aerogels with outstanding thermal insulating capacity, which is essential to provide infrared stealth and radar stealth for military equipment and to protect sensitive electronic devices from high-temperature attacks. This work offers a prospective strategy for constructing high-performance absorption-dominated EMI shielding materials with excellent thermal insulation properties, and the obtained aerogels present broad application prospects in the fields of aviation, portable electronic equipment and national defense industry.
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高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2021
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IF 3.927
Qiulian Li,Shizhong Sun,Xinyu Li,Xiang Li,Xiu Liu,Daoyong Zhang,Na Yu,Shurong Wang
Kesterite Cu 2 ZnSn(S,Se) 4 (CZTSSe) is emerging as one of the most promising materials owing to its low-cost, non-toxicity, similar electronic properties with Cu 2 (In,Ga)Se 2 (CIGS). However, the current highest power conversion efficiency (PCE) for CZTSSe device is far below the CIGS because of the high open-circuit voltage (V oc ) deficit and low fill factor (FF). Here, we fabricated CZTSSe thin film from 2-methoxyethanol solutions and investigated the effects of different Sn (Sn 2+ vs Sn 4+ ) oxidation states of precursor solution and selenization temperature on the crystal quality of the CZTSSe thin film and device performances. By characterizations and analyses, we found that incomplete redox reaction caused by the off-stoichiometric component in Sn 2+ precursor solution led to the formation of detrimental secondary phases such as SnSe, Cu 2 Se, and SnSe 2 in the CZTSSe thin film. The existence of volatile SnSe could cause the formation of voids and thus affected the FF and V oc . The reaction from Sn 4+ precursor solution to absorber material avoided the formation of SnSe. Ultimately, the Sn 4+ thin film showed better features in terms of improving crystal quality and reducing V oc deficit that limited the efficiency of kesterite CZTSSe thin film solar cells. Besides, we demonstrated that an appropriate selenization temperature could further reduce the number of secondary phases and improve the surface morphology and crystallinity of the CZTSSe thin film. As a result, we obtained CZTSSe thin film solar cells with 8.27% PCE from the Sn 4+ precursor solution under the selenization temperature of 580 °C.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 19
·6498-6506
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IF 6.119
Shengxin Chen,Ran An,Yingwei Li,Yuting Zhu,XinBao Zhu,Ruixia Liu,Xingang Li
Although poly(ionic liquid)s (PILs) have received extensive attention and research, the strategy for designing efficient PILs catalysts remains a challenge. This work reports a series of efficient PILs catalysts with increasing ionic ratio and various anion species to regulate electrophilic/nucleophilic ability, and explores the effect of the ionic ratio on the coupling reaction of propylene oxide (PO) with CO2 or methanol. These PILs are synthesized by a quaternization reaction between poly(N-vinylimidazole) (PVIM) and dihaloalkanes, where the amount of crosslinker of dihaloalkanes controls the ionic ratio of PILs, further affecting their microcosmic environment, morphologies and properties. It is noteworthy that the ionic ratio with IL units and imidazoline group can work as a trigger and promoter in the coupling reaction of PO with CO2 or methanol. The ionic ratio could open the reaction compared with the parent PVIM and the choice of anion could turn the reaction on or off. It suggested that the active microstructure and electrophilic/nucleophilic ability of PILs could be regulated by the ionic ratio. In these active sites, the IL units-connected imidazoline group could weaken the interaction of the cation–anion, giving enhanced leaving ability of the anion, contributing to the excellent catalytic performance.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Guijun Li,Yibo Tang,Tiantian Fu,Yang Xiang,Zhongping Xiong,Yujun Si,Chaozhong Guo,Zhiqiang Jiang
The development of efficient and cost-effective bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for the commercialization of rechargeable metal-air batteries. Herein, the pyrolysis of a precursor containing g-C 3 N 4 , thiourea, cobalt chloride and ferric chloride was used to fabricate S, N co-doped carbon nanotubes functionalized with Co 3 Fe 7 alloy nanoparticles (CoFe/S-N-C). The obtained CoFe/S-N-C catalyst exhibited an ORR half wave potential of 0.855 V ( vs . RHE) in 0.1 M KOH, outperforming a commercial Pt/C catalyst ( E 1/2 = 0.844 V). The catalyst also demonstrated superior OER catalytic activity (1.588 V at 10 mA cm −2 ) relative to RuO 2 in 0.1 M KOH, thus displaying outstanding bifunctional ORR and OER activity. A rechargeable Zn-air battery fabricated using CoFe/S-N-C shows good very performance (maximum power density of 120 mW cm −2 with a specific capacity of 814 mAh g −1 ) which was superior to a Zn-air battery fabricated using Pt/C and RuO 2 as ORR and OER catalysts (92 mW cm −2 and 787 mAh g −1 , respectively). Further, the fabricated battery using CoFe/S-N-C showed good stability, offering a discharge voltage ∼ 1.10 V and a recharge voltage ∼ 2.15 V at 10 mA cm −2 over 300 cycles, evidence of the durability of the CoFe/S-N-C catalyst.
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Acta Pharmaceutica Sinica B
·
2021
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IF 11.614
Boyi Niu,Yixian Zhou,Kaixin Liao,Ting Wen,Sixian Lao,Guilan Quan,Xin Pan,Chuanbin Wu
The therapeutic efficacy of cisplatin has been restricted by drug resistance of cancers. Intracellular glutathione (GSH) detoxification of cisplatin under the catalysis of glutathione S -transferases (GST) plays important roles in the development of cisplatin resistance. Herein, a strategy of “pincer movement” based on simultaneous GSH depletion and GST inhibition is proposed to enhance cisplatin-based chemotherapy. Specifically, a redox-responsive nanomedicine based on disulfide-bridged degradable organosilica hybrid nanoparticles is developed and loaded with cisplatin and ethacrynic acid (EA), a GST inhibitor. Responding to high level of intracellular GSH, the hybrid nanoparticles can be gradually degraded due to the break of disulfide bonds, which further promotes drug release. Meanwhile, the disulfide-mediated GSH depletion and EA-induced GST inhibition cooperatively prevent cellular detoxification of cisplatin and reverse drug resistance. Moreover, the nanomedicine is integrated into microneedles for intralesional drug delivery against cisplatin-resistant melanoma. The in vivo results show that the nanomedicine-loaded microneedles can achieve significant GSH depletion, GST inhibition, and consequent tumor growth suppression. Overall, this research provides a promising strategy for the construction of new-type nanomedicines to overcome cisplatin resistance, which extends the biomedical application of organosilica hybrid nanomaterials and enables more efficient chemotherapy against drug-resistant cancers.
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PubMed
高影响因子
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