Journal of Energy Chemistry
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2023
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IF 13.1
Tong Dou,Jinqing He,Shuteng Diao,Yiping Wang,Xuhui Zhao,Fazhi Zhang,Xiaodong Lei
As the “emission peak and carbon neutrality peak” are proceeding all over the world, CO 2 electroreduction is studied extensively as it is a powerful way to transform CO 2 into value-added products. The earth-abundant Sn-based materials and copper sulfides as electrochemical catalysts have shown activity for generating formate from CO 2 electroreduction. Herein, the composite of CuS and S-doped SnO 2 (CuS/SnO 2 -S) was synthesized by a redox reaction under room temperature. The unique structural reconstruction of CuS/SnO 2 -S nanoparticles to Cu/Sn/Cu 6.26 Sn 5 nanowires decreases the energy barrier of the adsorption of CO 2 , and increases the adsorption of *H, primarily suppressing the competing reaction of hydrogen evolution reaction (HER). As a result, at − 0.8 V vs. RHE , it reaches an electrochemical CO 2 -to-formate conversion with a Faradaic efficiency (FE) of 84.9% at a yield of 8860 µmol h −1 cm − 2 under a partial current density of ∼18.8 mA cm − 2 in an H-type reactor. This study provides significant insight into the structural evolution of the CuSn sulfides and the mechanism of formate formation.
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PEST MANAGEMENT SCIENCE
·
2023
·Vol. 79
·期 8
·2725-2736
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IF 4.1
Qi Li,Ning Zhao,Minghao Jiang,Mali Wang,Jingxu Zhang,Haiqun Cao,Min Liao
BACKGROUND Echinochloa glabrescens Munro ex Hook. f. is one of the main Echinochloa spp. seriously invading Chinese rice fields and has evolved resistance to commonly used herbicides. Previously, an E. glabrescens population (LJ-02) with suspected resistance to the acetyl-CoA carboxylase (ACCase)-inhibiting herbicide metamifop was collected. This study aimed to determine its resistance status to metamifop and investigate the internal molecular mechanisms of resistance. RESULTS Single-dose testing confirmed that the LJ-02 population had evolved resistance to metamifop. Gene sequencing and a relative expression assay of ACCase ruled out target-site based resistance to metamifop in LJ-02. Whole-plant bioassays revealed that, compared with the susceptible population XZ-01, LJ-02 was highly resistant to metamifop and exhibited cross-resistance to fenoxaprop- P -ethyl. Pretreatment with the known glutathione S -transferase (GST) inhibitor, 4-chloro-7-nitrobenzoxadiazole (NBD-Cl), largely reversed the resistance to metamifop by approximately 81%. Liquid chromatography–tandem mass spectrometry analysis indicated that the metabolic rates of one of the major metabolites of metamifop, N -(2-fluorophenyl)-2-hydroxy- N -methylpropionamide (HPFMA), were up to 383-fold faster in LJ-02 plants than in XZ-01 plants. There were higher basal and metamifop-inducible GST activities toward 1-chloro-2,4-dinitrobenzene (CDNB) in LJ-02 than in XZ-01. Six GST genes were metamifop-induced and overexpressed in the resistant LJ-02 population. CONCLUSION This study reports, for the first time, the occurrence of metabolic metamifop resistance in E. glabrescens worldwide. The high-level metamifop resistance in the LJ-02 population may mainly involve specific isoforms of GSTs that endow high catalytic activity and strong substrate specificity. © 2023 Society of Chemical Industry.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
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IF 6.2
Lufang Fan,Jiahui Han,Kai Wei,Changchang Ma,Sheng Feng,Yun Zhou,Xiaojun Dai,Zhiwei Ye,Yang Wang
This study aimed to regulate the band structure and enhance the reduction ability of CdS by substituting it with Mn 2+ . Subsequently, this nano MnCdS solid solution was anchored on the surface of truncated octahedral Cu 2 O through a simple hydrothermal process, forming an S-scheme heterojunction at the interface between MnCdS and Cu 2 O. Equilibrating the Fermi level at the MnCdS/Cu 2 O heterojunction led to spontaneous diffusion of electrons in MnCdS to Cu 2 O, generating an internal electric field that drove the recombination of electrons in the conduction band (CB) of Cu 2 O and holes in the valence band (VB) of MnCdS. Consequently, this process preserved the powerful photogenerated electrons in the CB of MnCdS, facilitating robust photocatalytic hydrogen evolution . The MnCdS/Cu 2 O exhibited a photocatalytic hydrogen evolution rate of 66.3 mmol g −1 h −1 , which was 3.4- and 54.3-times higher than that of MnCdS (19.4 mmol g −1 h −1 ) and Cu 2 O (1.2 mmol g −1 h −1 ), respectively. This study elucidates advanced S-scheme heterojunction catalyst architectures for photocatalytic hydrogen production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Zhipeng Mao,Wei Hao,Wei Wang,Fubin Ma,Chengcheng Ma,Shougang Chen
As an influential antifouling material, photocatalytic materials have drawn attention increasingly over recent years owing to their potential bacteriostatic property in the domain of marine antifouling. Herein, a flower-like BiOI@CeO 2 @Ti 3 C 2 S-scheme photocatalyst was contrived and prepared by hydrothermal method . The innovative combination of Ti 3 C 2 and narrow band gap semiconductor BiOI was implemented to modify CeO 2 and the photocatalytic bacteriostatic mechanism of BiOI@CeO 2 @Ti 3 C 2 was elucidated. Schottky junction was formed between CeO 2 and Ti 3 C 2 , and a p-n junction was formed between CeO 2 and BiOI. By photoelectrochemical characterization, BCT-10 exhibits the best photoelectrochemical performance of which photogenerated carrier transport can be performed more readily at 10 % CeO 2 @Ti 3 C 2 addition. 99.76 % and 99.89 % of photocatalytic bacteriostatic efficiency of BCT-10 against Escherichia coli and Staphylococcus aureus were implemented respectively, which were 2.98 and 3.07 times higher than that of pure CeO 2 . The ternary heterojunction can suppress photogenerated electron-hole complexes more effectively and enhance the photocatalytic bacteriostatic effect of CeO 2 , which also provided a new concept to the further broadened application of CeO 2 in the marine bacteriostatic and antifouling field.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2023
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IF 5.8
Qiang Huang,Zhiren Zou,Xiaobo Li,Qinwen Xiao,Guang Liang,Wenqi Wu
The drug-amino acid co-amorphous systems and amorphous solid dispersions (ASDs) are promising methods to address the poor water solubility of poorly water-soluble drugs. However, some amino acids might not be perfect co-formers for co-amorphous systems, and the relatively low drug-loading of many ASDs is one of the main disadvantages of ASDs. Thus, poly- l -lysine and polyglutamic acid were selected as the co-formers, ball milled with basic mebendazole, neutral tadalafil and acidic valsartan at different weight ratios (from 3:1 to 1:3) to prepare poly (amino acid)-based ASDs, aiming to combine the advantages of co-amorphous systems (high drug-loading) and ASDs (relatively high T g and high physical stability). All the mixtures were converted into amorphous after milling. The powder dissolution studies showed that drug-poly (amino acid) ASDs improved the dissolution rate of the drug in different ways and to different degrees. Moreover, the two poly (amino acid)s enhanced the physical stability of amorphous drugs. It is worthy to mention that the salt formation between the drug and the poly (amino acid) does not necessarily mean better performance compared to non-salt forming systems, and salt formation is also not a prerequisite for the formation of promising drug-poly (amino acid) ASDs.
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CHEMISTRY-A EUROPEAN JOURNAL
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2023
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IF 4.3
Bingrong Wang,Nan Zhang,Yifeng Wang,Delun Chen,Junlei Qi,Jinchun Tu
Graphical Interface construction through experimental control of the introduced anions allows the tuning of the energy bands of photoanode materials. The cooperative energy band and electronical structure of In 2 O 3 /In 2 S 3 resulted in a photocurrent of 0.6 mA⋅cm −2 when exposed to light irradiation. This strategy has practical significance for developing low-cost, high-performance PEC sensors. In the past several decades, Photoelectrochemical (PEC) sensing still remains a great challenge to design highly-efficient semiconductor photocatalysts via a facile method. It is of much importance to design and synthesize various novel nanostructured sensing materials for further improving the response performance. Herein, we present an In 2 O 3 /In 2 S 3 heterostructure obtained by combining microwave assisted hydrothermal method with S-induced phase change, whose energy band and electronic structure could be adjusted by changing the S content. Combining theoretical calculation and spectroscopic techniques, the introduction of sulfur was proved to produce multifunctional interfaces, inducing the change of phase, oxygen vacancies and band gap, which accelerates the separation of photoexcited carriers and reduces their recombination, improving the electronic injection efficiency around the interface of In 2 O 3 /In 2 S 3 . As anticipated, an enhanced glucose response performance with a photocurrent of 0.6 mA cm −2 , a linear range of 0.1–1 mM and a detection limit as low as 14.5 μM has been achieved based on the In 2 O 3 /In 2 S 3 heterostructure, which is significant superior over its pure In 2 O 3 and S-doped In 2 O 3 counterparts. This efficient interfacial strategy may open a new route to manipulate the electrical structure, and energy band structure regulation of sensing material to improve the performance of photoelectrodes for PEC.
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Nanoscale
·
2022
·Vol. 14
·期 39
·14520-14528
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IF 8.307
Weiwei Xu,Ningbo Fan,Shiji Xu,Linxing Meng,Bin Xu,Min Zhou,Wei Tian,Liang Li
Introducing suitable interfacial chemical bonds into heterojunctions can increase the charge carrier density, propel the charge separation, and facilitate interfacial charge extraction in photoanodes for photoelectrochemical (PEC) water oxidation. However, tuning chemical bonds at heterojunction interfaces and elucidating their influences on band alignment and the associated evolution of PEC performance remain elusive. Herein, Bi–S bonds were introduced into the interface of a CdIn2S4 (CIS)/Bi2WO6 (BWO) heterojunction. In situ irradiated X-ray photoelectron spectroscopy and electron spin resonance signals confirm that the Bi–S bond transforms the band alignment from type II to the direct Z-scheme, significantly enhancing the carrier separation efficiency. Theoretical calculations show that the Bi–S bond not only acts as an atomic-level charge transfer channel, but also changes the migration pathway and distance within the heterojunction. As a result, the optimized CIS/BWO photoanode exhibits a relatively high PEC performance of 4.25 mA cm−2 at 1.23 V vs. RHE (VRHE) and a low onset potential of 0.30 VRHE. This work presents a new avenue to construct comprehensively improved photoanodes by tuning the interfacial structures at the atomic level.
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Nanomaterials
·
2022
·Vol. 12
·期 21
·3770
·
IF 5.719
Ruowei Yi,Yinchao Zhao,Chenguang Liu,Yi Sun,Chun Zhao,Yinqing Li,Li Yang,Cezhou Zhao
The nitrogen-doped MXene carbon nanosheet-nickel (N-M@CNi) powder was successfully prepared by a combined process of electrostatic attraction and annealing strategy, and then applied as the separator coating in lithium–sulfur batteries. The morphology and structure of the N-M@CNi were characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), Raman spectrum, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption–desorption method. The strong LiPS adsorption ability and high conductivity are associated with the N-doped carbon nanosheet-Ni modified surface. The modified separator offers the cathode of Li–S cell with greater sulfur utilization, better high-rate adaptability, and more stable cycling performance compared with the pristine separator. At 0.2 C the cell with N-M@CNi separator delivers an initial capacity of 1309 mAh g−1. More importantly, the N-M@CNi separator is able to handle a cathode with 3.18 mg cm−2sulfur loading, delivering a capacity decay rate of 0.043% with a high capacity retention of 95.8%. Therefore, this work may provide a feasible approach to separator modification materials towards improved Li-S cells with improved stability.Keywords:MXene;carbon nanosheets;lithium–sulfur batteries;modified separator
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ChemistrySelect
·
2022
·Vol. 7
·期 40
·e202203024
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IF 2.307
Xuehui You,Fang Liu,Guofei Jiang,Shuhua Chen,Beiya An,Rongli Cui
Graphical Degradation experiments of TC suggested that SCN/NT-2@PTFE composites showed the best photocatalytic performance under the optimal conditions, the degradation rate of tetracycline reached 99 % after 120 min of irradiation. The preparation of SCN/NT-2@PTFE composite membrane can solve the problem of difficult recovery and secondary contamination of powder catalysts. Herein we synthesized S-g-C 3 N 4 and N−TiO 2 catalysts by hydrothermal and calcination technologies and SCN/NT@PTFE membrane by a vacuum filtration method. The morphology and composition of the synthesized materials were analyzed by different characterization methods (SEM/HRTEM/XRD/XPS/UV-vis et.). The effects of different catalysts, pollutant concentrations, mass of catalyst and pH on the photo-degradation of tetracycline were investigated. The degradation rate of tetracycline by SCN/NT-2@PTFE membrane was as high as 99.9 % after 2 h of illumination. This was mainly because heterogeneous structure between S-g-C 3 N 4 and N−TiO 2 broadened the light absorption range and suppressed the carrier complex. Superoxide radicals (⋅O 2 − ) were proved to play a dominant role in the degradation reaction. After 20 days of stirring in water, the photocatalytic performance of membrane decreased slightly, demonstrating its good stability. The study of SCN/NT-2@PTFE membrane provides a new direction for the development of photocatalysis and membrane.
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POLYMER
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2022
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IF 4.432
Zhen Wang,Shu Feng Zhou,Yi Zhi Zhuo,Ao Nan Lai,You Zhong Lu,Xiao Bin Wu
Current anion exchange membranes (AEMs) for fuel cells suffer from low ionic conductivity and poor mechanical property. Herein, we introduce adamantane groups onto the block poly(arylene ether sulfone)s backbone to form the selected comb-shaped structure. The structure-property relationships of the AEMs are investigated by varying the ratio of the hydrophobic to hydrophilic segments. The bulk rigid adamantane group can restrain the swelling of the AEMs thus enhancing the mechanical properties and expand the spacing between the hydrophilic/hydrophobic segments of the polymer chains to promote the formation of microphase separation morphology. Consequently, as characterized by atomic force microscope (AFM) and transmission electron microscopy (TEM), the resulting membranes show well-defined microphase separation between the hydrophilic/hydrophobic segments, resulting in high ionic conductivity range from 27.4 to 90.2 mS cm −1 over a temperature range of 30–80 °C. At the same time, the membranes present ultralow swelling ratio with the levels from 1.6% to 6.1% at 30 °C and from 6.8% to 12.7% at 80 °C, respectively, and thus excellent mechanical properties with the tensile strength as high as 11.52 MPa and elongation at break of 29.28%. The excellent comprehensive properties grant the prepared AEMs bright future for fuel cells.
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ANALYST
·
2022
·Vol. 147
·期 16
·3675-3683
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IF 5.227
Chunyu Gao,Ziyi Ding,Jiangkun Tan,Jinmao You,Zan Li
Studies have shown that homocysteine (Hcy) levels are closely related to cardiovascular and cerebrovascular diseases. In this work, we have developed and synthesized three copper complexes, F542-Cu2+, F508-Cu2+, and F465-Cu2+ for Hcy detection. The different binding constants (Ks) of the copper complexes endow them with dramatic reactivity toward biothiols. The pyridine-containing tetraazacycle was employed in the construction of F542-Cu2+, which renders the medium Ks value for the copper complex compared with cyclen and TACN and effectively prevented the disintegration of the complexes. Pyridine-containing tetraazacycle provided the basis and possibility for the hypothesis for the reduction of Cu2+ by biothiols to shape into a stable six-membered ring structure. The obtained results verified that F542-Cu2+ could be utilized to specifically probe Hcy in a switched-on fluorescence mode. F542-Cu2+ exhibited excellent environmental stability, superior sensitivity, and outstanding selectivity toward Hcy under physiological conditions. The mechanism of Hcy specificity was confirmed to be related to the generation of Hcy-induced six-membered ring by fluorescence imaging, time-dependent fluorescence spectra, ESI-MS, and electron paramagnetic resonance (EPR) analyses. Furthermore, we exploited the application of F542-Cu2+ and developed a strategy for evaluating the activity of S-adenosylhomocysteine hydrolase (AHCY) in vitro by fluorescence analysis. More importantly, real-time in vivo evaluation of the enzymatic activity of AHCY was realized and assisted by our probe, providing the possibility of opening up a new avenue for enzymatic reaction assessment.
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MACROMOLECULES
·
2022
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IF 6.057
Gaopeng Shi,Xiaoning Geng,Yuanbiao Liu,Guozhang Wu
Enthalpy hysteresis (ΔHR), an easily accessible quantity determined from a well-defined cooling and subsequent heating cycle of heat capacity curves, was recently reported to bear a proportional relationship with the α-related excess entropy of polymers at glass transition temperature( Tg). The kinetic fragility m of polymers was thus verified to link with thermodynamic parameters of Tg·ΔCp/ΔHR, as predicted by the Adam–Gibbs equation. In this work, enthalpy hysteresis of poly(n-alkyl methacrylate)s was investigated systematically to clarify whether ΔHR is influenced by multifarious non-α-related contributions. The results showed that the ΔHR for higher poly(n-alkyl methacrylate)s is abnormally suppressed, as manifested by failure of the theoretic correlation between m and Tg·ΔCp/ΔHR. The anomalous suppression appears non-related to the βJG relaxation but stems from nanophase separation of the alkyl sidechains. Once the PE-like nanophase is completely destroyed, either by increasing the steric hindrance of side groups or by introducing small molecule-bridged hydrogen bonds, ΔHR recovers, and the theoretic correlation between m and Tg·ΔCp/ΔHR is re-established. Further experiments revealed that the abnormal ΔHR suppression occurs only when the periodicity of phase separation is comparable to the size of the cooperative rearrangement region of bulk α relaxation at Tg. Accordingly, the deviation of m and Tg·ΔCp/ΔHR correlations from the theoretic prediction must be related to the existence of two different but partly coupled glass transitions in higher poly(n-alkyl methacrylate)s. The extremely hindered and confined glass transition in the PE-like nanodomains is likely to cause the anomalous suppression of global enthalpy hysteresis.
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