Inorganic Chemistry Frontiers
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2025
·
IF 6.4
Kexin Yang,Zhijia Song,XiaoXiao Fu,Wei Yan,Tao Zhang,Yiwei Hua,Haixin Lin,Qin Kuang,Zhaoxiong Xie
The photocatalytic direct one-step two-electron (2e-) oxygen reduction reaction (ORR) holds great potential in efficient H2O2 synthesis. However, it is still a significant challenge to design photocatalysts for achieving high-efficiency H2O2 production via this direct one-step 2e- ORR pathway. To address this, we have constructed a Z-scheme BAIO/C3N4 heterojunction by in situ growing Ba2AgIO6 (BAIO) on the surface of C3N4 nanosheets. Under visible light irradiation, the optimal sample, with a BAIO:C3N4 mass ratio of 1:1.5, exhibited a remarkable H2O2 yield of up to 535.9 μmol g-1 h-1, which is 8.8 times higher than that of pure C3N4. This enhancement is attributed to the improved charge separation and migration efficiency facilitated by the enhanced internal electric field (IEF) in BAIO/C3N4 heterojunction. Furthermore, the heterojunction altered the O2 adsorption configuration to the Yeager-type, promoting a more efficient and selective direct one-step 2e- ORR for H2O2 production. This study highlights the importance of regulating the reaction pathway to enhance photocatalytic H2O2 production activity and offers a new insight for designing highly active photocatalysts.
研究领域:
光催化
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材料科学
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环境科学
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能量转换
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化学反应工程
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DOI
高影响因子
GREEN CHEMISTRY
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2025
·
IF 9.2
Yongji Xia,Sheng Lin,Jian Yan,Renjie Xu,Yingpeng Du,Chunxiao Song,Dong-Liang Peng,Zhidong Zhou,Jiajia Han,Guanghui Yue
Spinel-type Co3O4 has been identified as a highly prospective cathode catalyst for lithium-oxygen batteries (LOBs), attributable to its distinctive bimetallic active sites that manifest exceptional bifunctional catalytic characteristics. Nonetheless, the practical implementation of this process is constrained by the inherent conductivity limitations of Co3O4 and the suboptimal utilization of active sites. In this study, a Cu-Mn bimetallic doping strategy is employed to prepare a spherical-like structure of Co3O4 formed by self-assembling one-dimensional nanorods. The introduction of Cu²⁺ results in a reduction of the surface energy of the system, thereby facilitating the directional growth of the nanorods. The redox-active Mn³⁺/Mn⁴⁺ pairs exhibit an inhibitory effect on Ostwald ripening, achieved by stabilizing the fine particles during synthesis and regulating solute diffusion kinetics. This combined action of Cu and Mn enhances active site exposure and optimizes charge transfer kinetics. Furthermore, the doping of bimetallic ions resulted in the redistribution of the Co3+/Co2+ ratio, optimizing the electronic structure for efficient charge transfer during the reaction. The combination of tailored electronic states and optimized nanostructures demonstrates excellent dual-functional catalytic activity for ORR and OER, with a half-wave potential of 0.71 V (vs RHE) for OER and an overpotential of 400 mV (10 mA cm-2) for ORR. The assembled LOBs can be stably cycled up to 450 cycles and an ultra-high discharge capacity of 7268 mAh g-1 for LOBs. This study provides a novel reference for the design of efficient bifunctional catalysts.
研究领域:
材料科学
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电化学
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储能技术
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纳米材料
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催化
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DOI
高影响因子
Journal of the American Chemical Society
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2017
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IF 13.858
Shuai Xu,Peng Zhou,Zehui Zhang,Changjun Yang,Bingguang Zhang,Kejian Deng,Steven Bottle,Huaiyong Zhu
Selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is one of the key reactions for producing chemical commodities from biomass and their derivatives. The challenge for this reaction is to develop an efficient catalytic process that can be conducted under mild conditions (room temperature and atmospheric pressure, using oxygen molecules in air as the oxidant) and a recyclable catalyst. Herein we report a photocatalyst of cobalt thioporphyrazine (CoPz) dispersed on g-C3N4 (abbreviated as CoPz/g-C3N4), which exhibits excellent catalytic activity toward the selective oxidation of HMF into FDCA under simulated sunlight using oxygen molecules in air as a benign oxidant. For example, an FDCA yield of 96.1% in an aqueous solution at pH = 9.18 is achieved at ambient temperature and air pressure. At lower pH (4.01), the product generated is 2,5-diformylfuran. Hence, it is possible to control the reaction outcome by control of the pH of the reaction system. g-C3N4 itself is not a suitable catalyst for the selective oxidation because under the experimental conditions g-C3N4 generates hydroxyl radicals that initiate processes that oxidize HMF directly to CO2 and H2O. CoPz on the other hand activates O2 to give singlet oxygen (1O2), which more controllably oxidizes HMF to FDCA albeit at a more moderate yield (36.2%). The strong interaction between the CoPz and g-C3N4 in the CoPz/g-C3N4 catalyst is experimentally evidenced, which not only improves accessibility of the CoPz sites and makes the catalyst recyclable but also disables the hydroxyl radical generation by g-C3N4 and promotes 1O2 generation on the CoPz sites, significantly enhancing the catalytic performance. This study demonstrates the potential for efficient non-noble metal photocatalysts for organic transformations driven by sunlight.
研究领域:
化学工程
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催化科学
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环境科学
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DOI
高影响因子
Small Methods
·
2022
·Vol. 6
·期 6
·2200178
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IF 15.367
Rui Xu,Phei Er Saw,Lei Xu
Two-dimensional (2D) nanomaterials have attracted increasing attention in cancer theranostics due to their ultrahigh specific surface area resulting in more radicals and/or reactive oxygen species (ROS) generation in chemodynamic therapy (CDT). However, their biomedical prospects are greatly limited by poor biocompatibility, low dispersion, weak stability, and the potential threat of their high immunogenicity. Moreover, rapid depletion of ROS by the high level of antioxidants (e.g., glutathione) in cancer cells severely limits the therapeutic effects of cancer CDT. Herein, a robust method is developed to improve the biomedical application of 2D nanomaterials via constructing a 2D nanomaterials delivery nanoplatform with hemoglobin-based minerals biological coat for the safe encapsulation, long blood circulation, and controlled release of 2D nanomaterials. After intravenous administration and then internalization by cancer cells, the acidic microenvironment and high concentration of H 2 O 2 can trigger rapid release of Cu-T nanoscale metal-organic frameworks (nMOFs) from Cu-T@MH. Then, the released Cu-T nMOFs with simultaneous high ROS production and GSH depletion endow the Cu-T@MH nanoplatform with enhanced cancer CDT. Besides, the fluorescence recovery of tetrakis(4-carboxyphenyl) porphyrin in Cu-T nMOFs during the GSH depletion process can accurately visualize the cancer therapeutic action.
研究领域:
生物医学工程
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肿瘤学
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纳米医学
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2017
·Vol. 27
·期 43
·1700626
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IF 12.124
Chi Zhang,Wei-Hai Chen,Li-Han Liu,Wen-Xiu Qiu,Wu-Yang Yu,Xian-Zheng Zhang
Conventional photodynamic therapy (PDT) has limited applications in clinical cancer therapy due to the insufficient O 2 supply, inefficient reactive oxygen species (ROS) generation, and low penetration depth of light. In this work, a multifunctional nanoplatform, upconversion nanoparticles (UCNPs)@TiO 2 @MnO 2 core/shell/sheet nanocomposites (UTMs), is designed and constructed to overcome these drawbacks by generating O 2 in situ, amplifying the content of singlet oxygen ( 1 O 2 ) and hydroxyl radical (•OH) via water-splitting, and utilizing 980 nm near-infrared (NIR) light to increase penetration depth. Once UTMs are accumulated at tumor site, intracellular H 2 O 2 is catalyzed by MnO 2 nanosheets to generate O 2 for improving oxygen-dependent PDT. Simultaneously, with the decomposition of MnO 2 nanosheets and 980 nm NIR irradiation, UCNPs can efficiently convert NIR to ultraviolet light to activate TiO 2 and generate toxic ROS for deep tumor therapy. In addition, UCNPs and decomposed Mn 2+ can be used for further upconversion luminescence and magnetic resonance imaging in tumor site. Both in vitro and in vivo experiments demonstrate that this nanoplatform can significantly improve PDT efficiency with tumor imaging capability, which will find great potential in the fight against tumor.
研究领域:
癌症治疗
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纳米技术
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生物医学工程
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光化学
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成像技术
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DOI
高影响因子
Catalysts
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2026
·Vol. 16
·期 4
·364
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IF 4.5
Lihui Wang,Shao Zhang,Mingming Wang,Zhigang Wang,Xiaoyao Tan
The high-temperature proton ceramic membranes with simultaneous separation of hydrogen and oxygen exhibit promising applications in the catalytic conversion field. However, their separation performance often relies on external electrical circuits, which limits practical application. To overcome this limitation, doping strategies have emerged as a viable approach to develop triple-conducting (H+/e−/O2−) membranes for simultaneous hydrogen and oxygen separation in non-electrochemical mode. In this study, honeycomb-structured hollow fiber membranes were fabricated, and the effects of varying Fe3+and Y3+doping concentrations on hydrogen and oxygen permeation fluxes were systematically investigated. At the Fe3+doping level of 0.2 mol, the oxygen permeation flux of 0.692 mL min−1cm−2in BaCe0.6Zr0.2Fe0.2O3−δ(BCZF) was achieved at 1000 °C, while the hydrogen permeation flux was 0.201 mL min−1cm−2. The BaCe0.55Fe0.05Zr0.2Y0.2O3−δ(Fe-BCZY) hollow fiber membrane can enhance the hydrogen permeation flux by 75% at 1000 °C. Furthermore, during the simultaneous permeation of hydrogen and oxygen, a 1.7-fold enhancement in hydrogen permeation performance was achieved for the Fe-BZCY hollow fiber membrane at 1000 °C, and with oxygen permeation flux of 1.76 mL min−1cm−2at the same temperature. More significantly, a hydrogen permeation flux of 0.34 mL min−1cm−2can be achieved at 700 °C under simultaneous hydrogen and oxygen permeation, which is favorable for the application of membrane reactors in catalytic reactions.
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DOI
高影响因子
Batteries-Basel
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2023
·Vol. 9
·期 5
·
IF 4
Ningning Feng,Chaoqiang Wang,Jing Wang,Yang Lin,Gang Yang
Lithium–oxygen (Li-O2) batteries have captured worldwide attention owing to their highest theoretical specific energy density. However, this promising system still suffers from huge discharge/charge overpotentials and poor cycling stability, which are related to the leakage/volatilization of organic liquid electrolytes and the inefficiency of solid catalysts. A mixing ionic liquid-based gel polymer electrolyte (IL-GPE)-based Li-O2battery, consisting of a 20 mM 2,5-di-tert-butyl-1,4-benzoquinone (DBBQ) 40 mM N-methylphenothiazine (MPT)-containing IL-GPE and a single-walled carbon nanotube cathode, is designed for the first time here. This unique dual redox mediators-based GPE, which contains a polymer matrix immersed with mixed ionic liquid electrolyte, provides a proper ionic conductivity (0.48 mS cm−1) and effective protection for lithium anode. In addition, DBBQ, as the catalyst for an oxygen reduction reaction, can support the growth of discharge products through the solution–phase pathway. Simultaneously, MPT, as the catalyst for an oxygen evolution reaction, can decompose Li2O2at low charge overpotentials. Hence, the DBBQ-MPT-IL-GPE-based Li-O2battery can operate for 100 cycles with lower charge/discharge overpotentials. This investigation may offer a promising method to realize high-efficiency Li-O2/air batteries.
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2026
·
IF 6
Chaosi Liu,Yijing Gao,Yixiang Niu,Yumei Zhang,Cheng Wang,Tengda Li,Chunhui Xu,Weidong Zhu,Xinqing Lu
Develop Pd-based catalysts for propylene epoxidation with H 2 and O 2. • Sn species in PdSn/Ti-MWW increase the electron density of Pd. • Increased electron density of Pd enhances the H 2 utilization. • Sn significantly promotes the catalytic propylene epoxidation. The low-temperature epoxidation of propylene with H 2 and O 2 to propylene oxide (PO), commonly referred to as the low-temperature HOPO process, over titanosilicate zeolite-supported Pd catalysts is economically attractive and environmentally friendly. However, PO selectivity remains a major challenge for these systems and is comparatively low, because this process is commonly accompanied with propylene hydrogenation to propane. In the present study, a novel and efficient Ti-MWW-supported PdSn catalyst (PdSn/Ti-MWW) was developed for this low-temperature HOPO process, displaying a substantially high PO selectivity. The results on extensive characterizations, in combination with Density Functional Theory (DFT) calculations, for PdSn/Ti-MWW and Pd/Ti-MWW verify that the introduction of Sn species into Pd/Ti-MWW can boost the electron density of Pd species while does not affect the coordination states of Ti species and the textural properties of the zeolite. Interestingly, the enhanced Pd electron density will weaken the adsorption of propylene on the Pd active sites, resulting in inhibiting propylene hydrogenation, which is beneficial for the selective production of PO. Catalytic tests reveal that the optimal 0.33Pd0.22Sn/Ti-MWW catalyst achieves a PO selectivity of 68.4 % and a maximum PO productivity of 7.5 mol g Pd -1 h −1 , far exceeding monometallic Pd/Ti-MWW, while the undesired propane selectivity drops sharply. Moreover, PdSn/Ti-MWW shows an excellent stability and reusability as key catalytic traits. Thus, this work establishes an effective electronic modulation strategy for designing high-performance bimetallic Pd catalysts, and lays solid experimental and theoretical foundations for the industrial application of sustainable low-temperature HOPO technology. Download: Download high-res image (81KB) Download: Download full-size image
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高影响因子
ChemSusChem
·
2023
·
IF 8.4
Juanjuan Han,Yangyang Zhang,Xiumeng Zheng,Yuyang Lu,Wanting Li,Xiaorong Zhou,Zhandong Ren,Yi Liu,Meixue Hu,Li Xiao,Lin Zhuang
Graphical A novel AEM with good strength and flexibility was synthesized by combining rigid PPO and flexible PVA. Dual cationic groups were added to improve ion concentration and create ion channels, enhancing ion conductivity. Cross-linking and phase separation improved the AEM's resistance to alkali. A series of cross-linked AEMs ( c -DQPPO/PVA) are synthesized by using rigid polyphenylene oxide and flexible poly(vinyl alcohol) as the backbones. Dual cations are grafted on the PPO backbone to improve the ion exchange capacity (IEC), while glutaraldehyde is introduced to enhance compatibility and reduce swelling ratio of AEMs. In addition to the enhanced mechanical properties resulting from the rigid-flexible cross-linked network, c -DQPPO/PVA AEMs also exhibit impressive ionic conductivity, which can be attributed to their high IEC, good hydrophilicity of PVA, and well-defined micro-morphology. Additionally, due to confined dimension behavior and ordered micro-morphology, c -DQPPO/PVA AEMs demonstrate excellent chemical stability. Specifically, c -DQPPO/PVA-7.5 exhibits a wet-state tensile strength of 12.5 MPa and an elongation at break of 53.0 % at 25 °C. Its OH − conductivity and swelling degree at 80 °C are measured to be 125.7 mS cm −1 and 8.2 %, respectively, with an IEC of 3.05 mmol g −1 . After 30 days in a 1 M NaOH solution at 80 °C, c -DQPPO/PVA-7.5 experiences degradation rates of 12.8 % for tensile strength, 27.4 % for elongation at break, 14.7 % for IEC, and 19.2 % for ion conductivity. With its excellent properties, c -DQPPO/PVA-7.5 exhibits a peak power density of 0.751 W cm −2 at 60 °C in an H 2 -O 2 fuel cell.
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产品关联
DOI
PubMed
高影响因子
Carbon Energy
·
2023
·
IF 20.5
Feiyang Yang,Ying Yao,Yunkai Xu,Cong Wang,Meiling Wang,Jingjie Ren,Cunzhong Zhang,Feng Wu,Jun Lu
Although biomass-derived carbon (biochar) has been widely used in the energy field, the relation between the carbonization condition and the physical/chemical property of the product remains elusive. Here, we revealed the carbonization condition's effect on the morphology, surface property, and electrochemical performance of the obtained carbon. An open slit pore structure with shower-puff-like nanoparticles can be obtained by finely tuning the carbonization temperature, and its unique pore structure and surface properties enable the Li–O 2 battery with cycling longevity (221 cycles with 99.8% Coulombic efficiency at 0.2 mA cm −2 and controlled discharge–charge depths of 500 mAh g −1 ) and high capacity (16,334 mAh g −1 at 0.02 mA cm −2 ). This work provides a greater understanding of the mechanism of the biochar carbonization procedure under various pyrolysis conditions, paving the way for future study of energy storage devices.
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DOI
高影响因子
Nano Research
·
2023
·Vol. 16
·期 5
·6278-6289
·
IF 9.9
Xu Jialun,Zhang Zhihua,Yu Daiyi,Du Wei,Song Nan,Duan Xuezhi,Zhou Xinggui
The catalytic performances over propylene epoxidation with H 2 and O 2 (HOPO process) are significantly affected by the properties (e.g., surface properties, Ti coordination, and morphology) of titanosilicate zeolite. Introducing urea into zeolite synthesis is a simple and convenient method to modify these properties of titanosilicate zeolite. Uncalcined pore-blocked titanium silicalite-1 (TS-1, i.e., TS-1-B) with the lower urea dosage possesses more defective structure and unsaturated coordinated Ti sites verified by 29 Si nuclear magnetic resonance (NMR) and X-ray photoelectron spectroscopy (XPS) analysis, which results in a high initial activity and hydrogen efficiency; while the high surface acidity generated by these Ti species leads to a continuous decrease in the activity and the propylene oxide (PO) selectivity during the reaction. As the amount of urea gradually increases, the TS-1-B samples present the reduced surface defects and defective and unsaturated Ti species. Specially, TS-1-B-0.30U presents the weaker PO adsorption on PO-diffusion reflectance infrared Fourier transform spectra (DRIFTS), and thus results in the high stable PO formation rate and selectivity over its Au catalyst. Furthermore, a flat-plate-like shape with a shorter thickness of 100 nm along the b-axis direction is observed on the urea-modified TS-1. Compared with the conventional ellipsoidal TS-1 with crystal sizes of 200 and 500 nm, the flat-plate-like TS-1-0.30U displays the less surface defects, unsaturated Ti species, and the weaker Lewis acid, which is favorable for the desorption and intracrystalline diffusion of PO, thus reduces the occurrence of side reactions for the improved selectivity and stability. This work may provide a reference for developing titanium-containing materials with high activity and stability over HOPO reaction.
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高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Zhongxi Xie,Shuang Liang,Xuechao Cai,Binbin Ding,Shanshan Huang,Zhiyao Hou,Ping’an Ma,Ziyong Cheng,Jun Lin
Hypoxia and overexpression of glutathione (GSH) are typical characteristics of the tumor microenvironment, which severely hinders cancer treatments. Here, we design a novel biodegradable therapeutic system, O2–Cu/ZIF-8@Ce6/ZIF-8@F127 (OCZCF), to simultaneously achieve GSH depletion and O2-enhanced combination therapy. Notably, the doped Cu2+ doubles the O2 storage capacity of the ZIF-8 matrix, which makes OCZCF an excellent pH-sensitive O2 reservoir for conquering tumor hypoxia, enhancing the photodynamic therapy (PDT) efficiency of chlorin e6 (Ce6) under 650 nm laser irradiation. Moreover, the released Cu2+ can act as a smart reactive oxygen species protector by consuming intracellular GSH. The byproduct Cu+ will undergo highly efficient Fenton-like reaction to achieve chemodynamic therapy (CDT) in the presence of abundant H2O2. The accompanying O2 will further alleviate hypoxia. The in vitro and in vivo experimental data indicate that OCZCF could cause remarkable tumor inhibition through enhanced synergetic PDT and CDT, which may open up a new path for cancer therapy.
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DOI
PubMed
高影响因子
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