Journal of Energy Chemistry
·
2024
·
IF 14
Dong Zhang,Minghui Zhu,Ran Qin,Peixian Chen,Maoye Yin,Dafeng Zhang,Junchang Liu,Hengshuai Li,Xipeng Pu,Peiqing Cai
Rational design of photocatalyst to maximize the use of sunlight is one of the issues to be solved in photocatalysis technology. In this study, the CuFe 2 O 4 @C/Cd 0.9 Zn 0.1 S (CFO@C/CZS) S-scheme photocatalyst with photothermal effect was synthesized by ultrasonic self-assembly combined with calcination. The dark CFO@C absorbed visible light and partly converted into heat to promote the hydrogen evolution reaction. The presence of heterojunctions inhibited the photogenerated electron-hole recombination. The graphite-carbon layer provided a stable channel for electron transfer, and the presence of magnetic CFO made recycle easier. Under the action of photothermal assistance and heterojunction, the hydrogen evolution rate of the optimal CFO@C/CZS was 80.79 mmol g −1 h −1 , which was 2.55 times and 260.61 times of that of pure CZS and CFO@C, respectively. Notably, the composite samples also exhibit excellent stability and a wide range of environmental adaptability. Through experimental tests and first-principles simulation calculation methods, the plausible mechanism of photoactivity enhancement was proposed. This work provided a feasible strategy of photothermal assistance for the development of heterojunction photocatalysts with distinctive hydrogen evolution.
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Cell Reports
·
2023
·
IF 8.8
Xue Wen,Yang Xiao,Haitao Xiao,Xueqin Tan,Beiyi Wu,Zehua Li,Ru Wang,Xuewen Xu,Tao Li
Summary Bisphenol S (BPS) exposure has been implied epidemiologically to increase obesity risk, but the underlying mechanism is unclear. Here, we propose that BPS exposure at an environmentally relevant dose aggravates diet-induced obesity in female mice by inducing brown adipose tissue (BAT) whitening. We explored the underlying mechanism by which KDM5A-associated demethylation of the trimethylation of lysine 4 on histone H3 (H3K4me3) in thermogenic genes is overactivated in BAT upon BPS exposure, leading to the reduced expression of thermogenic genes. Further studies have suggested that BPS activates KDM5A transcription in BAT by binding to glucocorticoid receptor (GR) in an estrogen-dependent manner. Estrogen-estrogen receptors facilitate the accessibility of the KDM5A gene promoter to BPS-activated GR by recruiting the activator protein 1 (AP-1) complex. These results indicate that BAT is another important target of BPS and that targeting KDM5A-related signals may serve as an approach to counteract the BPS-induced susceptivity to obesity.
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PubMed
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POLYMER SCIENCE SERIES B
·
2021
·Vol. 63
·期 4
·358-366
·
IF 1.049
Danbo Mao,Yuechuan Wang
Abstract Four 2,5-dicholorobenzoate monomers were prepared by chlorination and esterification and then polymerized to ester substituted poly( p -phenylene)s through Ni/Zn catalyzed coupling reaction. The thermal stability and pyrolysis behavior of ester substituted poly( p -phenylene)s were investigated through TGA method. The possible mechanism of thermal modification of the polymers was proposed that included de-esterification, dehydration and decarboxylation, and finally de-anhydridization. Only pyrolysis of esters substituted poly( p -phenylene)s containing two neighboring carboxyl groups may result in the formation of the corresponding anhydride.
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Journal of the American Chemical Society
·
2019
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IF 14.695
Cheng-Jian Zhang,Tian-Cheng Zhu,Xiao-Han Cao,Xin Hong,Xing-Hong Zhang
The synthesis of poly(thioether), a highly desired sulfur-containing polymer, is still a key challenge. Herein, we report a simple and facile approach to poly(thioether)s by closed-system one-pot reaction of carbonyl sulfide (COS) and epoxides. This route underwent the coupling reaction of COS with epoxides, followed by decarboxylative ring-opening polymerization (ROP) of the generated mixed cyclic thiocarbonates with releasing of CO2 and a little bit of COS. Organic base was used as catalyst and initiator in the two steps, respectively. The oxygen/sulfur exchange reaction was driven by successive regioselective elementary reactions and spontaneous releasing of CO2 (COS), leading to the sulfur atom of COS transferring to poly(thioether)s, which was well demonstrated by DFT studies. This work provides an easy-to-handle, metal-free route to poly(thioether)s bearing diverse structures by using readily available chemicals.
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PubMed
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MINERALS ENGINEERING
·
2022
·
IF 5.479
Xing-fu Zheng,Jin-lan Xia,Hong-chang Liu,Zhen-yuan Nie,Chang-qin Qin,Yu Wang,Jian-hua Chen
Elemental sulfur (S 0 ), as one of the most important intermediates formed during chalcopyrite bioleaching, can exist in a variety of allotropic forms, among which amorphous μ-S and orthorhombic ɑ-S 8 are the most common forms. Although previous studies have focused on the effect of S 0 on chalcopyrite bioleaching, how S 0 allotropes affect chalcopyrite bioleaching is unclear. Therefore, in this work, the differential effect of ɑ-S 8 and μ-S on chalcopyrite bioleaching by Acidithiobacillus ferrooxidans ( A. ferrooxidans ) was studied at the molecular and atomic levels by combining synchrotron radiation-based X-ray absorption near edge structure (XANES) spectroscopy, comparative transcriptome analysis and density functional theory (DFT) calculations, accompanied by the determination of solution behaviors and mineral surface morphologies. The results showed that µ-S was favorable for bacterial adsorption and that the addition of µ-S could promote the copper extraction rates by A. ferrooxidans , while the addition of ɑ-S 8 inhibited the copper extraction rates. The XANES results showed that both cases with the addition of ɑ-S 8 and µ-S could affect the formation and evolution of secondary minerals during bioleaching by A. ferrooxidans . The comparative transcriptome analysis showed that the gene expression of A. ferrooxidans was much more affected by the addition of µ-S, with more genes upregulated than ɑ-S 8 . The DFT results indicated that both ɑ-S 8 and µ-S could adsorb on the CuFeS 2 (0 0 1) surface easily, and µ-S could make the CuFeS 2 surface obviously change, while ɑ-S 8 hindered the adsorption of bacterial cells. Of note, µ-S could enhance the interaction between the CuFeS 2 (0 0 1) surface and bacterial cells with stronger bonding and more transferred electrons than ɑ-S 8 .
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ACS Biomaterials Science & Engineering
·
2023
·
IF 5.8
Lili Yu,Liyuan Xie,Zhengpeng Chen,Hongyun Guo,Yongdong Zhang,Haijun Wang,Rong Wang,Xing Zhou,Ziqiang Lei,Dedai Lu
Noninterventional embolization does not require the use of a catheter, and the treatment of solid tumors in combination with thermal ablation can avoid some of the risks of the surgical procedure. Therefore, we developed an efficient tumor microenvironment-gelled nanocomposites with poly [(l-glutamic acid-ran-l-tyrosine)-b-l-serine-b-l-cysteine] (PGTSCs) coated-nanoparticles (Fe3O4&Au@PGTSCs), from which the prepared PGTSCs were given possession of pH response to an acidic tumor microenvironment. Fe3O4&Au@PGTSC in noninterventional embolization treatment not only achieved the smart targeted medicine delivery but also meshed with noninvasive multimodal thermal ablation therapy and multimodal imaging of solid tumors via intravenous injection. It was worth noting that the results of animal experiments in vivo demonstrated that Fe3O4&Au@PGTSCs have specific tumor accumulation and embolization and thermal ablation effects; at 10 days postinjection, only scars were found at the tumor site. After 20 days, the tumors of model mice completely disappeared. This device is easier to treat solid tumors based on the slightly acidic tumor environment.
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PubMed
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Peizeng Yang,Jiating Liu,Gregory V. Korshin,Yuefei Ji,Junhe Lu
Tetrabromobisphenol S (TBBPS) is a brominated flame retardant and a contaminant of emerging concern. Several studies found that sulfate radical (SO4•–) oxidation is effective to degrade TBBPS. Here, we demonstrate that the presence of nitrite (NO2–) at environmentally relevant levels causes dramatic changes in the kinetics and pathways of TBBPS degradation by SO4•–. Initially, NO2– suppresses the reaction by competing with TBBPS for SO4•–. At the same time, SO4•– oxidizes NO2– to form nitrogen dioxide radicals (NO2•), which actively react with some key TBBPS degradation intermediates, thus greatly altering the transformation pathway. As a result, 2,6-dibromo-4-nitrophenol (DBNP) becomes the primary TBBPS product. As TBBPS undergoes degradation, the released bromide (Br–) is oxidized by SO4•– to form bromine radicals and free bromine. These reactive bromine species immediately combine with NO2• or NO2– to form nitryl bromide (BrNO2) that in turn attacks the parent TBBPS, resulting in its accelerated degradation and increased formation of toxic nitrophenolic byproducts. These results show that nitryl halides (e.g., BrNO2 or ClNO2) are likely formed yet inadequately recognized when SO4•– is applied to remediate halogenated pollutants in the subsurface environment where NO2– is ubiquitously found. These insights further underscore the potential risks of the application of SO4•– oxidation for the remediation of halogenated compounds in realistic environmental conditions.
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JOURNAL OF SUPERCRITICAL FLUIDS
·
2017
·
IF 2.991
Lei Bao,Shuyi Fang,Dongdong Hu,Ling Zhao,Weikang Yuan,Tao Liu
Four copolymers of vinyl acetate (VAc) and comonomers with different branched chains—dipropyl maleate (DPM), dibutyl maleate (DBM), diisobutyl fumarate (DiBF) and dineopentyl maleate (DNM)—were synthesised, and their CO 2 -philicity was evaluated by cloud point measurements. It was shown that poly(VAc-alt-DNM), containing the highest branched structure degree, had a 10% lower cloud point pressure at 40 °C than poly(VAc-alt-DBM)’s, the best CO 2 -philic hydrocarbon polymer available. Both ab initio calculations and molecular dynamics (MD) simulations showed that the highly branched structure weakened polymer–CO 2 interactions. However, the MD results for the cohesive energy density, solubility parameter, free volume fraction and radial distribution functions indicated that the more highly branched end groups contributed to an increase in the free volume fraction of the polymer, leading to low polymer–polymer interactions. Thus, the introduction of highly branched end groups into the polymer backbone was an efficient way to enhance the CO 2 -philicity of hydrocarbon polymers.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yanlin Pan,Dongliang Zheng,Jianxin Chen,Jun Zhou,Rui Wang,Xingyu Pan,Xiaobo Hu,Shaoqiang Chen,Pingxiong Yang,Jiahua Tao,Junhao Chu
The vapor transport deposition (VTD) processing is one of the most promising techniques to fabricate quasi-one-dimensional antimony selenosulfide (Sb 2 (S,Se) 3 ) photovoltaic materials with micrometer-scale grains and preferred crystal orientations . However, current researches rarely involve the effect of evaporation source on the film growth by VTD. Herein, we adopt Sb 2 (S,Se) 3 tablets as evaporation sources to develop Sb 2 (S,Se) 3 solar cells for the first time. We find that increasing the evaporation source area can effectively improve the deposition rate of Sb 2 (S,Se) 3 films, leading to an enhancement of the (221) preferred orientation and columnar large grains of the absorber layers, further improves the device photovoltaic performance . With fine-tuning of the evaporation source area, the optimized Sb 2 (S,Se) 3 solar cells show a high efficiency up to 7.6%. This study proposes a unique strategy to improving the quality of low-dimensional materials and a deeper understanding of the growth mechanism via vacuum methods.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 23
·期 3
·2005-2014
·
IF 3.43
Haibin Gou,Xifei Ma,Qian Su,Lei Liu,Ting Ying,Wei Qian,Li Dong,Weiguo Cheng
The development of metal-free, high effective and recyclable catalysts plays a pivotal role in transforming CO2 into high value-added products such as cyclic carbonates. In this paper, we introduced the hydrogen bond donor (HBD) groups into poly(ionic liquid)s via free radical polymerization, which successfully combined the HBD and ionic liquids (ILs) into one heterogeneous catalyst. The HBD could synergistically activate epoxides with hydroxyl functionalized ionic liquids and efficiently catalyze the cycloaddition of CO2 into cyclic carbonates. The yield of propylene carbonate (PC) reached 94% (at 105 °C, 2 MPa CO2, 3 h), which far exceeded poly(ionic liquid)s without HBDs functionalization (PC yield 72%), and even approached bulk ionic liquids (PC yield 95%). Moreover, HBD-functionalized poly(ionic liquid)s (HPILs) exhibited excellent recyclability after five runs and afforded wide substrate scope. According to the experimental results, 1H NMR spectra and density functional theory (DFT) calculations showed 2-hydroxyethyl methacrylate (HEMA) and the hydroxyl of ILs would form strong H-bonds with epoxides contributing to the ring-opening process of epoxides, and a possible HBD and nucleophilic anion synergistically catalytic mechanism was proposed. The method herein paved a brand new way for green technology and utilization of poly(ionic liquid)s.
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RSC Sustainability
·
2025
·
IF 4.9
Qianmeng Zhao,Shaifei Liu,Wen Liu,Mengqian Fu,Zhenyang Xu,Qian Su,Weiguo Cheng
Preparation of cyclic carbonates from CO2 and epoxides via cycloaddition is a well-established synthetic route, which is not only economical but also in line with the atomic economy. To overcome the problem of the cluster formation of hydrogen-bond donors in functionalized poly(ionic liquid)s, which reduces their catalytic activity, a series of spacer-functionalized poly(ionic liquid) catalysts were developed. In poly(ionic) liquids, the hydrogen-donating effect enhances the intrinsic catalytic performance of the active sites and the long-chain alkyl groups prevent interactions between hydrogen-bond-donor groups, thus increasing the utilization of the active sites. Among the developed poly(ionic liquid) catalysts, the poly(ionic liquid) P[AC12VIM][Br] containing amino groups demonstrated the highest catalytic activity (propylene oxide conversion up to 99%), which was comparable with that of bulky ILs. The best catalytic performance of P[AC12VIM][Br] was attributed owing to its multiple functions in not only activating CO2 and epoxides but also stabilizing Br−. Furthermore, the amphiphilicity of amino-functionalized poly(ionic liquid)s boosted their catalytic suitability for epoxide substrates with lipophilic edge groups, which was better than that of conventional poly(ionic liquid)s. Through XPS and NMR analyses, a mechanism of operation is proposed in which imidazole and hydrogen donor groups act co-operatively in epoxy during the reaction to assist in ring-opening. Thus, this study provides a new approach for improving the catalytic performance of poly(ionic liquid) catalysts from the viewpoint of an intrinsic reaction and utilization of the active sites.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Jing Liu,Hongxi Zhu,Lin Liu,Luliang Liao,Lingfang Qiu,Xun Xu,Youliang Shen,Ping Li,Xiaoyue Shi,Shuwang Duo
Nitrogen-defect-rich DCN enables Mn–N interfacial coupling with MnCo 2 S 4 . • Interfacial Mn–N bonding and S-scheme charge transfer promote efficient charge separation. • Enhanced ROS generation is achieved in the heterojunction under visible-light irradiation. • Optimized catalyst shows high visible-light activity and stability for TC degradation. • Degradation pathways and toxicity evolution demonstrate the deep mineralization and detoxification of TC. Constructing well-defined heterointerfaces is crucial for regulating charge separation and surface reactions in photocatalysts. Herein, MnCo 2 S 4 /g‑C 3 N 5 S-scheme heterojunctions were fabricated via an in-situ growth strategy, in which defect-associated nitrogen sites in g‑C 3 N 5 act as coordination centers to anchor Mn, forming well-defined Mn–N interfacial bonds. XANES/EXAFS analyses and density functional theory calculations confirm the presence of Mn–N coordination at the interface and reveal its role in tailoring the local coordination environment and electronic configuration of Mn. The Mn–N coupled heterointerface promotes directional separation and transfer of photogenerated carriers, as evidenced by photoelectrochemical measurements, electron spin resonance and femtosecond transient absorption spectroscopy, which demonstrate accelerated charge migration and enhanced generation of reactive oxygen species. Benefiting from this interfacial Mn–N bonding-driven charge separation, the optimized MnCo 2 S 4 /g‑C 3 N 5 -II heterojunction achieves markedly improved visible-light photocatalytic activity toward tetracycline degradation, reaching ~90.8% removal within 120 min with an apparent rate constant of 0.01371 min −1 , which far surpasses the individual components. This work highlights interfacial Mn–N bonding engineering as an effective strategy for constructing robust S-scheme heterojunctions with promoted charge separation and surface redox processes. Download: Download high-res image (182KB) Download: Download full-size image
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