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Energy Advances · 2024 · IF 3.2

An ultrathin Li-doped perovskite SEI film with high Li ion flux for a fast charging lithium metal battery

Ruliang Liu,Wenli Feng,Liangzhou Fang,Huiping Deng,Ling Lin,MinChang Chen,Jun-Xing Zhong,Wei Yin

Developing an artificial solid electrolyte interphase (SEI) with high Li ion flux is vital to improve the cycling stability of lithium metal batteries, especially under a high rate. In this work, a novel artificial SEI film was prepared via in situ deposition of a lithium-doped cesium lead chloride perovskite (Li–CsPbCl3). Benefiting from its ultra-high thickness (0.45 μm), high mechanical modulus (5.9 GPa), high lithium-ion migration number (0.57), and unique highly oriented framework, the Li–CsPbCl3 SEI film could promote the rapid transport and uniform deposition of lithium ions, enhancing the stability of lithium deposition and stripping. As a result, Li/Li symmetric cells based on the Li–CsPbCl3 protective film could cycle stably for 1300 hours under high current density of 10 mA cm−2. In addition, the Li/LiFePO4 battery using the Li–CsPbCl3 SEI film showed an impressive cycling stability with a capacity retention rate of up to 91.4% after 230 cycles at a high current rate of 3C.

研究领域: 材料科学 · 电化学 · 能源存储技术
✓ 已验证 DOI 高影响因子
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MICROCHIMICA ACTA · 2024 ·Vol. 191 ·期 3 ·1-11 · IF 5.3

Copper-zinc nanoparticle-decorated nitrogen-doped carbon composite for electrochemical determination of triclosan

Zhou Jie,Li Yaru,Li Yan,Lan Jing,Zhao Zongshan,Shi Rongguang

A new sensor based on copper-zinc bimetal embedded and nitrogen-doped carbon-based composites (CuZn@NC) was prepared for triclosan (TCS) detection by pyrolyzing the precursor of Cu–Zn binuclear metal–organic framework (MOF). The performance for detecting TCS was evaluated using linear scanning voltammetry (LSV) and differential pulse voltammetry (DPV), and the proton and electron numbers during TCS oxidation have been proved to be one-to-one. The results indicated that CuZn@NC can present a satisfactory analysis performance for TCS detection. Under the optimized conditions, the linear response range was 0.2–600 µM and the detection limit was 47.9 nM. The sensor presented good stability (signal current dropped only 2.5% after 21 days) and good anti-interference of inorganic salts and small molecular organic acids. The good recovery (97.5–104.1%) for detecting spiked TCS in commercial products (toothpaste and hand sanitizer) suggested its potential for routine determination of TCS in real samples. Graphical abstract

研究领域: 分析化学 · 环境科学 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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APPLIED AND ENVIRONMENTAL MICROBIOLOGY · 2017 ·Vol. 83 ·期 23 · IF 3.807

A Novel Aerobic Degradation Pathway for Thiobencarb Is Initiated by the TmoAB Two-Component Flavin Mononucleotide-Dependent Monooxygenase System in Acidovorax sp. Strain T1

Cui-Wei Chu,Bin Liu,Na Li,Shi-Gang Yao,Dan Cheng,Jia-Dong Zhao,Ji-Guo Qiu,Xin Yan,Qin He,Jian He

Thiobencarb is a thiocarbamate herbicide used in rice paddies worldwide. Microbial degradation plays a crucial role in the dissipation of thiobencarb in the environment. However, the physiological and genetic mechanisms underlying thiobencarb degradation remain unknown. In this study, a novel thiobencarb degradation pathway was proposed in Acidovorax sp. strain T1. Thiobencarb was oxidized and cleaved at the C—S bond, generating diethylcarbamothioic S-acid and 4-chlorobenzaldehyde (4CDA). 4CDA was then oxidized to 4-chlorobenzoic acid (4CBA) and hydrolytically dechlorinated to 4-hydroxybenzoic acid (4HBA). The identification of catabolic genes suggested further hydroxylation to protocatechuic acid (PCA) and finally degradation through the protocatechuate 4,5-dioxygenase pathway. A novel two-component monooxygenase system identified in the strain, TmoAB, was responsible for the initial catabolic reaction. TmoA shared 28 to 32% identity with the oxygenase components of pyrimidine monooxygenase from Agrobacterium fabrum, alkanesulfonate monooxygenase from Pseudomonas savastanoi, and dibenzothiophene monooxygenase from Rhodococcus sp. TmoB shared 25 to 37% identity with reported flavin reductases and oxidized NADH but not NADPH. TmoAB is a flavin mononucleotide (FMN)-dependent monooxygenase and catalyzed the C—S bond cleavage of thiobencarb. Introduction of tmoAB into cells of the thiobencarb degradation-deficient mutant T1m restored its ability to degrade and utilize thiobencarb. A dehydrogenase gene, tmoC, was located 7,129 bp downstream of tmoAB, and its transcription was clearly induced by thiobencarb. The purified TmoC catalyzed the dehydrogenation of 4CDA to 4CBA using NAD+ as a cofactor. A gene cluster responsible for the complete 4CBA metabolic pathway was also cloned, and its involvement in thiobencarb degradation was preliminarily verified by transcriptional analysis.IMPORTANCE Microbial degradation is the main factor in thiobencarb dissipation in soil. In previous studies, thiobencarb was degraded initially via N-deethylation, sulfoxidation, hydroxylation, and dechlorination. However, enzymes and genes involved in the microbial degradation of thiobencarb have not been studied. This study revealed a new thiobencarb degradation pathway in Acidovorax sp. strain T1 and identified a novel two-component FMN-dependent monooxygenase system, TmoAB. Under TmoAB-mediated catalysis, thiobencarb was cleaved at the C—S bond, producing diethylcarbamothioic S-acid and 4CDA. Furthermore, the downstream degradation pathway of thiobencarb was proposed. Our study provides the physiological, biochemical, and genetic foundation of thiobencarb degradation in this microorganism.

研究领域: 环境微生物学 · 分子生物学 · 生物化学
✓ 已验证 DOI 高影响因子
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY · 2020 ·Vol. 2020 ·期 7 ·626-630 · IF 2.529

Switchable Dielectric Behavior and Order-Disorder Phase Transition in a New Organic-Inorganic Hybrid Compound: (CH3NH3)4[InCl6]Cl

Min Li,Guan-Cheng Xu,Wen-Bo Xin,Yin-Qiang Zhang

Graphical The new organic-inorganic hybrid compound (CH 3 NH 3 ) 4 [InCl 6 ]Cl has been successfully synthesized by reaction of methylammonium with indium(III) chloride tetrahydrate. It undergoes a first-order phase transition accompanied with an obvious step-like dielectric switching. A new organic-inorganic phase transition material (CH 3 NH 3 ) 4 [InCl 6 ]Cl ( 1 ), has been successfully synthesized and characterized. The compound undergoes a reversible first-order phase transition at Curie temperature Tc=284 K, accompanied with a wide hysteresis of 12 K, which investigated by differential scanning calorimetry (DSC). The temperature dependence of the dielectric permittivity discloses an obvious step-like dielectric anomaly. Single crystal X-ray diffraction reveals that the order-disorder transition of the [InCl 6 ] 3– anion and the methylammonium cation were the main factor drove the phase transition from high temperature phase with the space group P 2/ m to low temperature phase with the space group P 2/ n . This finding indicates that In-based organic–inorganic hybrids compounds can be used to build phase transition materials, which broaden the way for exploring dielectric switching materials.

研究领域: 材料科学 · 晶体学 · 物理化学
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Synthesis of 3,5-dichlorobenzene isocyanate-derived β-cyclodextrin and 3,5-dimethyl phenyl isocyanate-derived β-cyclodextrin chiral stationary phases and their applications in the separation of chiral compounds

Shuai Lv,Chuanbao Ma,Hailin Cong,Youqing Shen,Bing Yu

β-Cyclodextrin (β-CD) has a unique three-dimensional structure and chemical properties, and has a strong chiral separation ability. In this study, we linked 3,5-dichlorobenzene isocyanate to β-cyclodextrin and named this newly synthesized molecule β-CD-DCIPI. 3,5-Dimethylbenzene isocyanate was attached to β-cyclodextrin and named β-CD-DPIC. A modified polymerization-induced colloidal aggregation (PICA) method and self-made silica sol were used to synthesize mesoporous silica microspheres with a particle size of 2.38 μm-5.51 μm. A green non-toxic diazoresin (DR) is used as a coupling agent, which is connected to the surface of silica microspheres through electrostatic interaction. After ultraviolet light irradiation, ionic bonds are transformed into covalent bonds, and a new chiral stationary phase with chiral separation properties (β-CD-DCIPI@SiO 2 and β-CD-DPIC@SiO 2 ) is constructed. This article first characterizes the properties of mesoporous silica microspheres and β-CD-DCIPI@SiO 2 and β-CD-DPIC@SiO 2 . Through reversed-phase high-performance liquid chromatography (RP-HPLC), the separation performance of two new chiral stationary phases in chiral compounds was explored and compared, and five chiral enantiomers were effectively separated.

研究领域: 化学 · 分析化学 · 材料科学
✓ 已验证 DOI 高影响因子
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ACS Food Science & Technology · 2021 · IF 0

Improvement of Conversion Efficiency from d-Glucose to d-Allulose by Whole-Cell Catalysts with Deep Eutectic Solvents

Xiaoyan Chen,Fan Wang,Shijie Liu,Qiang Yu,Wen Wang,Yu Zhang,Zhongming Wang,Zhenhong Yuan

The synthesis efficiency of d-allulose, an ideal sugar substitute and dietary supplement, from d-glucose with whole-cell catalysts was improved by three out of the four tested deep eutectic solvents (DESs) based on choline chloride (ChCl). The promotion effects on the product yields with increments of up to 2.6-fold were observed in reactions with the presence of DESs in the order ChCl/glycerol < ChCl/urea < ChCl/ethylene glycol. DES compositions displayed distinct influences, but all positive effects appeared in the reactions with low DES contents (1–10%). Higher DES contents produced negative effects, and 40% even totally suppressed the reaction. The enhancement of efflux of intracellular molecules was proved by an analysis of the nucleic acid and protein contents in the medium. DES assisted in the increase in cell membrane permeability rather than in the damage of cell wall integrity, accelerating quick contacts between the enzyme and substrate and improving the conversion rate.

研究领域: 化学工程 · 生物化学 · 食品科学
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Materials Today Energy · 2017 · IF 0

Surface-activation modified perovskite crystallization for improving photovoltaic performance

Guoqing Tong,Xinzheng Lan,Zihang Song,Guopeng Li,Huan Li,Linwei Yu,Jun Xu,Yang Jiang,Yun Sheng,Yi Shi,Kunji Chen

An improved vapor-phase deposition that leveraged the use of surface activation of PbI 2 film has been developed for modifying perovskite crystallization process . This was achieved by loading Cl − ligands on closely-packed PbI 2 particle film—a scaffold that allowed in situ formation of perovskite active layer . The introducing of Cl − ligands served the Cl-capped and thus electrostatically-charged PbI 2 nanoparticles showed improved colloidal stability in DMF , which facilitated the preparation of PbI 2 film. More importantly, during the process of CH 3 NH 3 I (MAI) deposition i.e. the growth of perovskite materials, the presence of three-dimensional Cl − ligand matrix favored the formation of dense perovskite film. Moreover, a desired release of chloride was also achieved, thus promote the rearrangement of the perovskite during the volume expansion process. This finally led to a PCE of PSCs exceeding 16.42% under AM 1.5 irradiation. Therefore, surface-activation with Cl-ligand matrix could provide guidelines for the morphology optimization and the perovskite devices performance enhancement.

研究领域: 材料科学 · 纳米科技 · 物理化学 · 能源材料 · 半导体器件 · 薄膜技术 · 光电转换
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Journal of the American Chemical Society · 2023 · IF 15

Transforming a Primary Li-SOCl2 Battery into a High-Power Rechargeable System via Molecular Catalysis

Guodong Chen,Wenda Li,Xiaofan Du,Chen Wang,Xuelian Qu,Xiangyu Gao,Shanmu Dong,Guanglei Cui,Liquan Chen

Li-SOCl2 batteries possess ultrahigh energy densities and superior safety features at a wide range of operating temperatures. However, the Li-SOCl2 battery system suffers from poor reversibility due to the sluggish kinetics of SOCl2 reduction during discharging and the oxidation of the insulating discharge products during charging. To achieve a high-power rechargeable Li-SOCl2 battery, herein we introduce the molecular catalyst I2 into the electrolyte to tailor the charging and discharging reaction pathways. The as-assembled rechargeable cell exhibits superior power density, sustaining an ultrahigh current density of 100 mA cm–2 during discharging and delivering a reversible capacity of 1 mAh cm–2 for 200 cycles at a current density of 2 mA cm–2 and 6 mAh cm–2 for 50 cycles at a current density of 5 mA cm–2. Our results reveal the molecular catalyst-mediated reaction mechanisms that fundamentally alter the rate-determining steps of discharging and charging in Li-SOCl2 batteries and highlight the viability of transforming a primary high-energy battery into a high-power rechargeable system, which has great potential to meet the ever-increasing demand of energy-storage systems.

研究领域: 电化学 · 能源材料 · 纳米催化 · 电池技术 · 分子工程
✓ 已验证 DOI 高影响因子
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WATER SCIENCE AND TECHNOLOGY · 2019 ·Vol. 80 ·期 5 ·902-910 · IF 1.624

Mesoporous TiO2/carbon catalytic ozonation for degradation of p-chloronitrobenzene

Qun W.,Jingnan Z.,Hong L.,Mengling L.,Xiaohui L.,Zhichao Y.,Tao H.,Pengyu W.

In this study, a mesoporous TiO 2 /carbon catalyst (TiO 2 /C) was prepared by a facile impregnation-carbonization approach to catalyze ozonation of p -chloronitrobenzene ( p -CNB). The catalyst was well characterized and the catalytic efficiency under various conditions was systematically evaluated. TiO 2 /C has a disordered mesostructure with a high specific surface area. 92.8% of p -CNB (2 μmol/L) can be degraded within 20 min in the TiO 2 /C/O 3 system in the presence of 1 mg/L O 3 , 100 mg/L catalyst, at pH = 5. Based on the evaluation of the effect of basic parameters, it could be deduced that the removal of p -CNB relied on the synthetic effect of catalysis by TiO 2 /C and the autocatalytic induction of p -CNB. The removal efficiency of p -CNB, the structure change and the leaching of Ti ions were also evaluated in five cycles, indicating TiO 2 /C is stable and recyclable for catalytic ozonation in water treatment.

研究领域: 环境科学 · 催化化学 · 水处理技术 · 材料科学 · 环境工程 · 纳米材料应用
✓ 已验证 DOI 高影响因子
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Corrosion Communications · 2024 · IF 0

PDA-modified sol-gel coating for long-lasting corrosion protection on Al alloy 3003

Zhiyuan Feng,Jiao Li,Keqi Huang,Guoqiang Liu,Huanhuan Bai,Xin Huang,Jun Qi,Zhengwei Tang,Penghai Xu,Xiaofei Yang,Zheng Qu,Guozhe Meng

Within the realm of corrosion protection methods for Al alloys, sol-gel technique has garnered increasing attention. However, conventional sol-gel methodologies cannot provide adequate long-lasting corrosion protection to Al alloys when exposed to chloride-rich solutions. This paper introduces an innovative approach to substantially augment the corrosion resistance of aluminum alloys through utilization of polydopamine (PDA)-modified sol-gel films. Effort was made to fabricate a PDA-modified sol-gel coating and a systematic investigation was conducted thereof. Long-term corrosion performance of this coating in 3.5 wt.% NaCl solution was evaluated through electrochemical impedance spectroscopy (EIS). Results show that the low-frequency impedance of the PDA-modified sol-gel coating remains significantly high at 7.9 × 10 5 Ω·cm 2 , even after 36 d of immersion in 3.5 wt.% NaCl medium, indicative of excellent protective properties. It notably surpasses low-frequency impedance of the unmodified coating, which registers at 2.5 × 10 4 Ω·cm 2 . The incorporation of PDA into the sol-gel coating, facilitated by adsorption and diffusion mechanisms, serves to fill micrometer- and nanometer-scale defects of the coating, thereby markedly enhancing their compactness. Furthermore, despite its modest thickness of 9 μm, the PDA-modified coating exhibits enduring corrosion protection capabilities.

研究领域: 材料科学 · 表面工程 · 腐蚀与防护 · 纳米材料 · 电化学
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WATER SCIENCE AND TECHNOLOGY · 2016 ·Vol. 74 ·期 1 ·276-286 · IF 1.064

Adsorptive removal of PPCPs by biomorphic HAP templated from cotton

Huang Bin,Xiong Dan,Zhao Tingting,He Huan,Pan Xuejun

Biomorphic nano-hydroxyapatite (HAP) was fabricated by a co-precipitation method using cotton as bio-templates and employed in adsorptive removal of ofloxacin (OFL) and triclosan (TCS) that are two representative pharmaceuticals and personal care products (PPCPs). The surface area and porosity, crystal phase, functional group, morphology and micro-structure of the synthesized HAP were characterized by Brunauer–Emmett–Teller isotherm, X-ray powder diffraction, Fourier transform infrared spectroscopy, scanning electron macroscopic and transmission electron microscopy. The effects of initial pH, ionic strength, initial concentration, contact time and temperature on the removal of PPCPs were studied in a batch experiment. The adsorption of OFL and TCS was rapid and almost accomplished within 50 min. Kinetic studies indicated that the adsorption process of OFL and TCS followed the pseudo-first-order and pseudo-second-order models, respectively. The Freundlich isotherm described the OFL adsorption process well but the adsorption of TCS fitted the Langmuir isotherm better. Thermodynamics and isotherm parameters suggested that both OFL and TCS adsorption were feasible and spontaneous. Hydrogen bond and Lewis acid–base reaction may be the dominating adsorption mechanism of OFL and TCS, respectively. Compared to other adsorbents, biomorphic HAP is environmentally friendly and has the advantages of high adsorption capacity, exhibiting potential application for PPCPs removal.

研究领域: 环境科学 · 材料科学 · 纳米技术 · 环境污染与控制 · 吸附材料
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Air stability enhancement and mechanism of Mg-Ca-hydride-based hydrolysis materials

Qin Huang,Ruijun Qian,Bingshou Gong,Habibullah,Ji Zhou,Xue Yao,Yao Wang,Yigang Yan,Yungui Chen,Chaoling Wu

Mg-Ca-hydride-based materials are ideal portable H 2 source owing to excellent hydrolysis properties. However, when exposed to air, there is an explosion risk and serious hydrolysis property degradation due to the reaction with steam in air. In this work, by adding 5 wt% expanded graphite, 8 wt% AlCl 3 and 5 wt% polyethylene glycol 1000, the H 2 yield of a 30 wt% Ca-Mg alloy hydride plate after 4 h air exposure (80 RH%, 25 °C) is increased to 2.3 times that of the original sample without any attenuation. Furthermore, when 15 wt% polyethylene glycol 1000 was added, the attenuation rate after 24 h air exposure is decreased by 43 %. The characterization results show that Ca 4 Mg 3 H 14 is more easily hydrolyzed than MgH 2 . First-principles calculations demonstrate that Ca 4 Mg 3 H 14 interacts with H 2 O molecules more strongly, owing to larger adsorption energy to H 2 O. By adding appropriate amounts of expanded graphite, AlCl 3 and polyethylene glycol 1000, combined with pressing technology, the direct contact between the material and air can be delayed. Simultaneously, the hydrolysis performance of the material itself can be improved contributed to destruction of the Mg(OH) 2 passivation layer by expanded graphite and AlCl 3 , thereby jointly enhancing the long-term storage performance. This work may advance the engineering application of Mg-Ca-based hydrolysis materials.

研究领域: 材料科学 · 无机化学 · 能源化学 · 氢能源 · 功能材料
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