CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
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
·
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
·
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
·
2022
·
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
·
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
·
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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Polymer Chemistry
·
2022
·Vol. 13
·期 35
·5082-5093
·
IF 5.364
Xingfeng Lei,Guo Xiong,Yuyang Xiao,Tianhao Huang,Xiangze Xin,Shuyu Xue,Qiuyu Zhang
Shape memory polymers (SMPs) show tremendous application prospect in various fields owing to their stimuli responsiveness. However, their application in the high value-added aerospace industry still remains a great challenge, since it is problematic to engineer SMPs with both ideal shape memory properties and high heat resistance as well as outstanding mechanical strength. Herein, by incorporating amide hydrogen bonding interactions into a robust imide polymer backbone, a series of poly(amide-imide) hybridization networks have been fabricated, showcasing superior shape memory behavior together with impressive thermal stability and high mechanical strength, with a Tg above 300 °C and a tensile strength up to 108.3 MPa. Among all polymers, m-3FPAI exhibits outstanding heat resistance, high mechanical strength, low moisture sensitivity, excellent shape memory property and prominent multiple shape memory tolerance. After six consecutive cycles, a Rf still above 98.5% with a Rr ranging from 97.8% to 100% was observed, making m-3FPAI a promising candidate to be used in aerospace application.
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Regenerative Biomaterials
·
2022
·
IF 5.763
Dou Jie,Yang Rong,Jin Xingxing,Li Pengfei,Han Xiao,Wang Lijuan,Chi Bo,Shen Jian,Yuan Jiang
Nitric oxide (NO) plays an important role in wound healing, due to its ability to contract wound surfaces, dilate blood vessels, participate in inflammation as well as promote collagen synthesis, angiogenesis and fibroblast proliferation. Herein, keratin was first nitrosated to afford S-nitrosated keratin (KSNO). As a NO donor, KSNO was then co-electrospun with polyurethane (PU). These as-spun PU/KSNO biocomposite mats could release NO sustainably for 72 h, matching the renewal time of the wound dressing. Moreover, these mats exhibited excellent cytocompatibility with good cell adhesion and cell migration. Further, the biocomposite mats exhibited antibacterial properties without inducing severe inflammatory responses. The wound repair in vivo demonstrated that these mats accelerated wound healing by promoting tissue formation, collagen deposition, cell migration, re-epithelialization and angiogenesis. Overall, PU/KSNO mats may be promising candidates for wound dressing.
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Journal of Energy Storage
·
2023
·
IF 9.4
Xing Chen,Haijun Tao,Yinhua Jiang,Shishi Li,Yuxin Liu,Kun Xie,Yuqiao Wang
P-doped S vacancy-rich NiCo 2 S 4 hollow microspheres (P-NiCo 2 S 4-x HMSs) were prepared by hydrothermal, sulfuration, and phosphorization methods. P doping and S vacancy dual defects can be simultaneously obtained during the phosphorization process. The dual defects can modulate the electron structure and create abundant electrochemical sites, boosting electron transfer and reaction kinetics. Theoretical calculations illustrated that the dual defects could reduce the adsorption energy of OH − and Mulliken charges of Ni atoms, in favor of OH − adsorption. The hollow construction can increase the specific surface area, promote ion diffusion, and alleviate the volume variation during charge/discharge processes. The specific capacity and rate capability of the P-NiCo 2 S 4-x HMSs electrode can reach up to 1146.0 C g −1 at 1 A g −1 and 61.8 % at 30 A g −1 , respectively. The P-NiCo 2 S 4-x HMSs electrode exhibited remarkable cycling stability with a 79.5 % capacity retention after 20,000 consecutive charge/discharge cycles. The assembled P-NiCo 2 S 4-x //AC hybrid supercapacitor manifested an infusive energy density of 62.7 Wh kg −1 at 867 W kg −1 .
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Materials
·
2021
·Vol. 14
·期 24
·7655
·
IF 3.623
Huaijiu Deng,Mattia Biesuz,Monika Vilémová,Milad Kermani,Jakub Veverka,Václav Tyrpekl,Chunfeng Hu,Salvatore Grasso
We report on an ultrarapid (6 s) consolidation of binder-less WC using a novel Ultrahigh temperature Flash Sintering (UFS) approach. The UFS technique bridges the gap between electric resistance sintering (≪1 s) and flash spark plasma sintering (20–60 s). Compared to the well-established spark plasma sintering, the proposed approach results in improved energy efficiency with massive energy and time savings while maintaining a comparable relative density (94.6%) and Vickers hardness of 2124 HV. The novelty of this work relies on (i) multiple steps current discharge profile to suit the rapid change of electrical conductivity experienced by the sintering powder, (ii) upgraded low thermal inertia CFC dies and (iii) ultra-high consolidation temperature approaching 2750 °C. Compared to SPS process, the UFS process is highly energy efficient (≈200 times faster and it consumes ≈95% less energy) and it holds the promise of energy efficient and ultrafast consolidation of several conductive refractory compounds.Keywords:tungsten carbide;ultrarapid consolidation;ultrahigh temperature flash sintering
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
You Wu,Yi Yang,Miaoli Gu,Chuanbiao Bie,Haiyan Tan,Bei Cheng,Jingsan Xu
Solar photocatalysis is a promising, green, and sustainable technique for the synthesis of H 2 O 2 . In this study, low-dimensional ZnO/ZnIn 2 S 4 S-scheme heterojunction photocatalysts are fabricated using electrostatic spinning and chemical bath deposition methods for the efficient photocatalytic production of H 2 O 2 . ZnO nanofibers loaded with 20 wt% ZnIn 2 S 4 exhibit a superior H 2 O 2 production rate of 928 μmol g −1 h −1 , which is more than four times higher than that seen in pristine hexagonal phase ZnO and ZnIn 2 S 4 . First-principles calculations and in-situ X-ray photoelectron spectroscopy reveal the charge separation and transfer mechanisms in the S-scheme heterojunction. The construction of the S-scheme heterojunction facilitates the spatial separation of charge carriers, and electrons and holes with higher redox abilities are retained. Photoelectrochemical and photoluminescence tests further show that the formation of an S-scheme heterojunction is beneficial for the separation of photoinduced charge carriers. Electrochemical tests and electron paramagnetic resonance measurements indicate that H 2 O 2 production is primarily via a two-step single-electron O 2 reduction path. This study provides a new approach for the construction of S-scheme heterojunction materials that can efficiently produce H 2 O 2 under solar irradiation.
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