Catalysis Science & Technology
·
2023
·Vol. 13
·期 24
·7046-7058
·
IF 5
Wei Jin,Dekang Liu,Liyuan Zhang,Qian Sun,Yishan Wang,Enzhou Liu,Xiaoyun Hu,Hui Miao
Titanium dioxide (TiO2), a conventional n-type semiconductor, was widely used in photocatalysis, electrocatalysis and photoelectrocatalysis due to its good UV absorption and stable physical and chemical properties. However, its wide band gap and low oxygen reaction (OER) activity limited its application in photoelectrochemical (PEC) water splitting. In this work, we successfully constructed type-II Sb2(S,Se)3@TiO2 core–shell heterojunctions. Antimony sulfide selenide (Sb2(S,Se)3) was a quasi-one-dimensional light-absorbing material with an adjustable band gap (1.1–1.8 eV), which broadened the TiO2 light absorption range and effectively promoted the photogenerated carrier separation, transportation and utilization. Of particular note, novel Sb2(S,Se)3 nanospheres (NSPs) (ca. 69 nm) were in situ grown inside the tubes attributed to the unique space-confinement effect of TiO2 nanotubes (NTs). The IPCE value for Sb2(S,Se)3@TiO2 at 734 nm was 10.808% compared to 0.030% for TiO2. The separation efficiency and injection efficiency increased from 2.48% and 31.62% to 4.90% and 36.48%, respectively. The onset potential was moved negatively by 60 mV, and the maximum photocurrent density of 1.53 mA cm−2 at 1.23 V vs. RHE was 13.9 times higher than that of TiO2 (0.11 mA cm−2). This work provided a new idea for the application of TiO2 in the field of PEC water splitting.
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MACROMOLECULAR BIOSCIENCE
·
2023
·
IF 4.6
Runhai Chen,Yu Xia,Zhifang Ma,Yue Ke,Qiang Shi,Fazly I. Ataullakhanov,Mikhail Panteleev
Excessive amounts of reactive oxygen species (ROS) cause various biological damages and are involved in many diseases, such as cancer, inflammatory and thrombotic complications, and neurodegenerative diseases. Thus, ROS-responsive polymers with inherent ROS scavenging activity and biodegradability are extremely needed for the efficient treatment of ROS-related diseases. Here, this work fabricates the amphiphilic diblock copolymer PEG-b-PBC via ring-opening polymerization (ROP) of phenylboronic acid ester conjugated cyclic carbonate monomer. The copolymer easily forms micelles (BCM) and scavenges ROS rapidly. BCM not only releases the delivered drug but degrades to produce the small molecules p-hydroxybenzyl alcohol (HBA) with anti-inflammatory capability in the presence of H 2 O 2 . BCM can reduce the oxidative stress of human umbilical vein endothelial cells (HUVEC) and the levels of inflammatory factors secreted by macrophages, showing antioxidative and anti-inflammatory activity. Finally, BCM exerts a significant capability to reduce the complications of inflammation and thrombosis in vivo. The biodegradable aliphatic poly(carbonate)s have the potential to be used for drug delivery systems (DDS) for diseases induced by reactive oxygen species.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Yuqing Hu,Puhui Deng,Wenying Wang,Linping Zhang,Yu Hou
Element doping and collaboration with other cocatalysts are two vital strategies to improve the photoelectrochemical properties and overcome the drawbacks of CdS for better photocatalytic performance. In this work, a series of manganese cadmium sulfides (MnxCd1–xS) were obtained by a solvothermal method. When x is equal to or greater than 0.3, MnxCd1–xS is composed of Mn–Cd–S sosoloid and MnS. Among all these MnxCd1–xS products, the Mn0.5Cd0.5S sample showed the best photocatalytic hydrogen production (5.99 mmol g–1 h–1). To further elevate the hydrogen production rate of Mn0.5Cd0.5S, four kinds of Ni-POMs were coupled with it as cocatalysts, and all these composite photocatalysts displayed enhanced performance. The highest efficiency was observed for 15-Ni4–Mn0.5Cd0.5S, which is up to 36.58 mmol g–1 h–1. Various characterizations indicated that Ni4P2W18, Mn–Cd–S sosoloid and MnS in the 15-Ni4–Mn0.5Cd0.5S composite form a double type-II heterojunction, which facilitates the separation and transfer of photogenerated carriers.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Keke Dong,Han Li,Chengjia Zhang,Man Zhou,Qian Liang,Yanan Wang,Zhongyu Li,Song Xu
Improving the stability and electron-hole separation efficiency of semiconductor photocatalysts has always been a hot topic in the field of catalysis. In the present study, a novel Cu 2-x S@Mn 0.3 Cd 0.7 S (Cu 2-x S@MCS) core-shell heterojunction has been constructed by the in-situ traditional hydrothermal reaction on the basis of hollow Cu 2-x S nanocubes. The optimized Cu 2-x S@MCS-2 photocatalyst with expanded light absorption exhibits excellent stability and a higher hydrogen evolution rate of 42.43 mmol g −1 h −1 , which is 2.3 times and more than 1400 times contrasting to the pure Mn 0.3 Cd 0.7 S and Cu 2-x S, respectively. Multiple characterizations and structure analysis revealed that the Cu 2-x S@MCS heterojunction possesses outstanding charge separation efficiency and a wider specific surface area which can provide abundant active sites. Furthermore, the mechanism of photocatalytic H 2 evolution for Cu 2-x S@Mn 0.3 Cd 0.7 S S-scheme heterojunction is also proposed. This work thus provides a favorable strategy to inhibit the photogenerated charge carrier recombination and drive highly efficient photocatalytic hydrogen generation by synthesizing photocatalyst with in situ core-shell structures.
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JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Xiaoqing Liu,Guangshe Li,Xin Zhang,Jinjiang Wu,Chuang Yu,Linfeng Peng,Dan Zhang,Liping Li
Vanadium-based compounds have earned incremental attention as cathode for aqueous zinc ion batteries (AZIBs) due to their ideal electrical conductivity , rich valence states and flexible crystal structures. Unfortunately, their storage mechanisms are confusing and not well-established, especially for nitride . Herein, we have constructed a cubic vanadium nitride and nitrogen/sulfur doped carbon composite (VN@N/S–C) as a cathode for AZIBs. An in-depth examination of ex-situ XRD and XPS reveal that the electrochemical reduction during the first discharge process promotes a structural transformation of cubic VN to layered Zn 3+ x (OH) 2 V 2 O 7 ·2H 2 O, thus permitting subsequent insertion of Zn 2+ in such layered structure. Ex-situ SEM studies of electrodes further identify a morphology change of nanoparticles to nanosheets , corresponding to VN and Zn 3+ x (OH) 2 V 2 O 7 ·2H 2 O, respectively. New storage mechanism-the electrochemical reduction combined with the contributions from Zn 2+ (de)intercalation, furnishes the VN@N/S–C cathode a high discharge capacity of 232 mA h g −1 after 400 cycles at 4 A g −1 and good rate performance (252 mA h g −1 at 6 A g −1 ). Even at a low temperature of 0 °C, the cathode still delivers an excellent capacity of 361 mA h g −1 after 300 cycles at 1 A g −1 . This study offers a hint to improve the understanding on cubic structure for AZIBs.
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Electrocatalysis
·
2023
·
IF 3.1
Zhao Hongyu,Zhang Hao,Huang Ruoyu,Wang Jianmin,Cai Jiajia,Hu Jing,Chen Zhijie,Li Yongtao,Li Haijin
Developing excellent electrocatalysts is a significant step in accelerating the widespread implementation of the electrochemical hydrogen evolution reaction (HER). MoS 2 is one of the promising alternatives to platinum-based catalysts, while its HER activity is far from Pt due to the lack of active sites. It is urgent to develop a novel strategy to activate the basal planes of MoS 2 for enhancing the HER activity. Herein, a facile hydrothermal method with a low-temperature H 2 O 2 etching method is developed to fabricate MoS 2 with O-doped and S-vacancy dual defects. The dual defects MoS 2 nanosheet demonstrates remarkable hydrogen evolution reaction (HER) activity, achieving 10 mA cm −2 with a small overpotential of around 143 mV in 0.5 M H 2 SO 4 . Graphical Abstract
Construct dual-defect MoS2 via a facile hydrothermal method and mild H2O2 etching process.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Jiali Mu,Guifa Long,Xiangen Song,Siquan Feng,Xingju Li,Qiao Yuan,Bin Li,Zheng Jiang,Li Yan,Yunjie Ding
The local coordination environment of central active sites plays a critical role in tuning the catalytic properties of heterogeneous single-metal-site catalysts (HSMSCs). However, carbon supports with inert surface properties provide weak interaction with the active sites, which hamper the effective modulation of the coordination structure of HSMSCs. Herein, this work shows that introducing N and S atoms into carbon support can modify the coordination environment of single-Rh-site and effectively improves the catalytic activity for the methanol carbonylation reaction. The synthesized Rh/AC-NS with single-Rh-site exhibits a high methanol conversion of 88% and a stable acetyl production rate of 2812 h −1 , in contrast with 1285 h −1 of Rh/AC without N- and S- functional groups, and meanwhile remarkably higher than those of Rh/AC-N and Rh/AC-S with only N- or S- functional group under the same mild reaction conditions. As revealed by the experimental result and density functional theory (DFT) calculations, the special combination of N- and S- functional groups offers favorable coordination configuration and also beneficial electronic structure for facilitated CH 3 I oxidative addition and CO insertion steps of single-Rh-site. This work offers new opportunities for rationally tuning the coordination structure of HSMSCs for heterogeneous catalysis.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Jian Gao,Gao Xu,Qifeng Liang,Xiaoxiang Xu,Hailong Wang,Shiyan Liu,Jun Ren,Zebo Fang,Shunhang Wei
g-C 3 N 4 usually acts as the oxidation counterpart for overall water splitting reactions in semiconductor heterojunctions. Due to the poor water oxidation ability of g-C 3 N 4 , it is difficult to achieve efficient photocatalytic overall water splitting over g-C 3 N 4 -based heterojunctions. In this work, one-dimensional (1D) LaNbON 2 with strong water oxidation ability is prepared for the first time, and combined with two-dimensional (2D) g-C 3 N 4 to form semiconductor heterojunction by electrostatic self-assembly. The results of surface states, theoretical calculations, band structures and chemical probes indicate that the 2D g-C 3 N 4 and the 1D LaNbON 2 are tightly bonded through the electrostatic attraction and form a S-scheme type semiconductor heterojunction. In the heterojunction, the 1D LaNbON 2 and the 2D g-C 3 N 4 work as oxidation and reduction counterpart, respectively. The built-in electric field at their heterointerfaces effectively accelerates carrier separation. Thereby the solar-driven photocatalytic overall water splitting rate of the optimal 2D g-C 3 N 4 /1D LaNbON 2 heterojunction is ∼ 3.3 times as much as that of the 2D g-C 3 N 4 .
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RSC Advances
·
2017
·Vol. 7
·期 80
·51001-51007
·
IF 3.108
Chun-Nan Zhu,Dong-Yun Zheng,Hui-Min Cao,Shan-Ying Zhu,Xiao-Jun Liu
Ternary I–III–VI nanocrystals (NCs) without toxic elements, such as Cu–In–S, are promising candidates for biolabeling and bioimaging due to their favorable biocompatibility. At present, it remains a tremendous challenge to directly synthesize high-quality Cu–In–S/ZnS core/shell NCs in aqueous solution at atmospheric pressure. Herein, a simple and reliable strategy that combines the hot-injection method and successive ion layer adsorption and reaction has been proposed to realize aqueous synthesis of fluorescent Cu–In–S/ZnS core/shell NCs. The growth of ZnS shell around Cu–In–S NCs not only improved the fluorescence quantum yield by several hundred times and to the value of 18%, but also effectively enhanced their fluorescence stability by protecting Cu+ in Cu–In–S core from being oxidized to Cu2+. The prepared Cu–In–S/ZnS core/shell NCs with bright and stable fluorescence were conjugated with wheat germ agglutinin and further applied to cancer cell imaging. This strategy here should open new avenues for aqueous synthesis of high-quality nanomaterials with the core/shell structure for broad biomedical applications.
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Nanoscale
·
2023
·Vol. 15
·期 31
·12961-12971
·
IF 6.7
Shuo Wang,Mengke Li,Gaojie Yan,Zhipeng Yang,Yuchao Guo,Xi Sun,Yue Wang,Yi Feng,Huili Ding,Xiaojie Zhang
Lithium–sulfur (Li–S) batteries are severely restricted for practical application due to the polysulfide shuttle effect, Li dendrites and thermal runaway. The use of PEO-based polymer composite electrolytes (PCEs) as an alternative strategy suffers from limited lithium-ion conductivity with deficient long-range transfer route. Herein, Li6.4La3Zr1.4Ta0.6O12 (LLZTO) nanoparticles modified with an in situ-synthesized zwitterionic covalent organic framework layer (denoted as LLZTO@HUT4) were introduced into PEO-based PCEs. Zwitterionic HUT4 modified the lithiophobic LiOH/Li2CO3 layer on the surface of LLZTO nanoparticles, which could notably promote Li+ ion transport for superior electrochemical performance of PCEs. Additionally, the intermediate layer HUT4 located between LLZTO and PEO could further improve the mechanical properties of electrolytes due to the enhanced inorganic/organic interface compatibility and intermolecular interaction. As a result, the obtained LLZTO@HUT4-15%/PEO electrolyte exhibited a competent ionic conductivity of 0.73 mS cm−1 with a Li+ transference number of up to 0.74 at 60 °C. The assembled S@CNT|LLZTO@HUT4-15%/PEO|Li coin cell delivered a considerable initial discharge capacity of 1018 mA h g−1 at 0.2 C, with approximately 92.1% capacity retention after 100 cycles, elucidating an obviously suppressed shuttle effect.
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Small
·
2023
·
IF 13.3
Pengpeng Jia,Yu Zou,Jiang Jiang
Development of wound dressing with robust antibacterial and repair-promoting activity has always been an urgent biomedical task during the past years. The therapeutic effect of current hydrogel dressings containing single bioactive agent like nanoparticle or gas is still unsatisfactory for the treatment of infected wound. Herein, a CuS/NO co-loaded hydrogel (CuS/NO Gel) is proposed, which is constructed by sequential polymerization, reduction, and S-nitrosylation of CuS hybrid hydrogel with disulfide bonds. These CuS/NO Gel patches show good mechanical stability, high photothermal activity and excellent biocompatibility. When being applied to treat infected wound, CuS/NO Gel can not only eliminate infection effectively by the synergistic effect of mild photothermal heating and boosted NO release in infection phase, but also promote vascularization and collagen deposition due to the synchronous supply of Cu ion nutrients and low concentration NO signaling molecules in wound repair phase. Compared to hydrogel dressings with individual active agent (CuS Gel or NO Gel), CuS/NO Gel exhibits better antibacterial and repair-promoting activity both in vitro and in vivo. Therefore, this CuS/NO Gel holds great promise in the future clinical treatment against infected wound.
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RSC Advances
·
2023
·Vol. 13
·期 50
·35689-35694
·
IF 3.9
Huandi Hou,Ting Wang,Baohuan Wang,Wenting Guo,Xiang Miao,Xin Liang
Co–Mo–S based catalysts have promising applications in both the hydrogen evolution reaction (HER) and hydrodesulfurization (HDS). Herein, Co–Mo–S catalyst and Co–Mo–S catalyst with and without NaBH4 modification have been successfully synthesized by a simple hydrothermal synthesis method. Co–Mo–S catalysts with NaBH4 modification show better catalytic activity towards both HDS and the HER. The phase purity, morphology, crystal structures and electron valence distribution of the catalysts with and without NaBH4 modification were studied by experimental characterizations and theoretical calculations. The catalysts without NaBH4 modification are mostly 2H-MoS2, while the catalysts without NaBH4 modification have 1T-MoS2, and 1T-MoS2 is exposed to more active sites, which will be conducive to the results of HDS performance of the catalyst. DFT calculations investigated the required activation energies of 1T-MoS2 and 2H-MoS2 for HDS and HER, respectively. The activation energy required for both HDS and H2 generation of 1T-MoS2 is significantly lower than that for the 2H-MoS2 structure.
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