ACS Catalysis
·
2024
·
IF 11.3
Long Cheng,Rong Wang,Wenzhe Si,Yanxi Deng,Junhua Li,Yue Peng
Cu-based catalysts leveraging Cu+/Cu0 active sites have emerged as pivotal for synthesizing essential hydrocarbons and alcohols in electrochemical CO2 reduction, such as ethylene and ethanol (C2 products). However, the dynamic reduction of Cu+ to Cu0 during electroreduction leads to site instability, resulting in diminished efficiency for CO2 conversion to C2 products. Herein, we introduced Si into CuO by the selective dissolution method, engendering Cu–O–Si units to stabilize the Cu+/Cu0 sites. The catalyst manifested good activity in CO2 electroreduction with an elevated Faradaic efficiency for C2 products reaching 81.9% at −100 mA/cm2. After ten cycles of electrochemical testing, the Cu+/Cu0 sites and performance exhibited no signs of degradation. The Si incorporation significantly improved the hybridization of O 2p and Cu 3d orbitals, thereby reinforcing the Cu–O bonds and stabilizing the Cu+/Cu0 sites, which was critical in promoting C–C coupling via decreasing the energy barriers for *OCCO formation and enhancing C2 product selection. The active Cu+ cations with unsaturated coordination contributed to the reaction stabilization, thereby improving the preservation of Cu2O metastable state.
研究领域:
电化学
·
催化
·
材料科学
·
能源转化
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhilei Guo,Guohua Jing,Sara A. Tolba,Chung-shin Yuan,Yu-Hua Li,Xiaowei Zhang,Zhiwei Huang,Huawang Zhao,Xiaomin Wu,Huazhen Shen,Wenjie Xia
Transition metal oxide (TMO)-decorated TiO 2 catalysts excel at low-temperature Hg 0 oxidation. However, TMOs are typically found in large nanoparticles (NPs), resulting in a lower atom utilization efficiency. The current paper presents the design of an Au single atom (SA)-doped Ti 4+ defected TiO 2 (Au SAC-Ti 1-x O 2 ) and investigations concerning the influence of an O-Au-O coordination environment on Hg 0 oxidation. Au SAC-Ti 1-x O 2 was designed using an O-Au-O coordination environment and the O-Au-O orbital interaction was elucidated using density functional theory (DFT). The enhanced oxidative capability of lattice oxygen atoms and the interaction between Hg 0 and oxygen atoms were investigated. The O-Au-O coordination environment containing Au SAC Ti 1-x O 2 was then synthesized and characterized using X-ray absorption fine structure (XAFS), X-ray photoelectron spectroscopy (XPS), etc. Finally, Hg 0 oxidation catalytic activity was determined. Due to the increasing population of Au-O antibonding orbital interactions in the valence band, the bond order of O-Au-O in Au SAC Ti 1-x O 2 decreased significantly, thereby enhancing the oxidation ability of its adjacent oxygen atoms. Au SA and ultra-small Au clusters coexisted on a Ti 1-x O 2 catalyst, and the Hg 0 -oxidation efficiency at 150–200 °C was 14 times and 1.5 times greater than those of TiO 2 and 0.1 % Au/TiO 2 , respectively. Furthermore, Au SAC Ti 1-x O 2 was more resistant to the inhibition of SO 2 and NO. It provides an efficient method for developing highly active SA catalysts for Hg 0 oxidation.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Mengqi Zhou,Guoqiang Sun,Shuang-Quan Zang
The society’s urgent demand for environmentally friendly, safe and low-cost energy storage devices has promoted the research of aqueous zinc-ion batteries. However, the uneven deposition of Zn ions on anodes will lead to the growth of the dendrite and reduce the Coulombic efficiency as well as the lifespan of the devices. Herein, we construct an O,N-dual functionalized carbon cloth current collector via a simple hydrothermal strategy, in which the oxygen-containing functional groups and the N heteroatoms can regulate the transmission and deposition of Zn ions, respectively. The proposed synergistic strategy ensures the uniform distribution of Zn ions on the surface of the Zn anode and inhibits the formation of dendrites. The symmetric cell based on the O,N-dual doped carbon cloth presents superior cycling stability (318 h) with a low voltage hysteresis (11.2 mV) at an areal capacity of 1 mAh cm −2 (20% depth of diacharge). Meanwhile, the appreciably low overpotential (16 mV) and high Columbic efficiency (98.2%) also demonstrate that the O,N-dual functionalized carbon cloth can be worked as a promising host for Zn ions deposition.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
Journal of Biomaterials and Tissue Engineering
·
2016
·Vol. 6
·期 1
·35-41
·
IF 1.287
Wang Kunjie,Wang Xingyu,Li Mingliang,Li Hongxia,Guan Feng,Zhang Deyi,Feng Huixia,Fan Haiyan
The oxygen doped photoluminescent carbon nanodots (O-CDs) were prepared in the presence of the acidic or alkaline solution. Microstructural images of the produced O-CDs were studied using a high-resolution transmission electron microscopy (HRTEM). Other chemical properties were characterized
using UV-Vis, XRD, fluorescence, FTIR, XPS. The size of these O-CDs exhibits excellent dispersibility with a narrow distribution range (1.5 nm–4.0 nm). Yellow fluorescence was observed for HCl-treated O-CDs, the blue for NaOH-treated O-CDs. The FTIR analysis indicates there are abundant
O–H, C=O, and C–O functional groups distributed on the surface of these O-CDs, rendering a great potential for the binding with the biological systems in the biosensing and bioimaging technologies.
研究领域:
材料科学
·
化学
·
生物医学工程
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DOI
高影响因子
Solid Fuel Chemistry
·
2022
·Vol. 56
·期 1
·37-44
·
IF 0.829
Wang Ruiyu,Sun Bingkang,Zhu Jiliang,Fan Xing
Abstract Nano γ-Al 2 O 3 support was prepared by sol-gel method, and the Mg 2 Si/γ-Al 2 O 3 catalyst was prepared by impregnation method from Mg 2 Si and the γ-Al 2 O 3 support. The catalyst was characterized by X-ray diffraction, N 2 adsorption-desorption, scanning electron microscopy and CO 2 temperature-programmed desorption analysis. The catalytic hydrocracking of lignite-related modelcompounds, 1-methoxynaphthalene (1-MON) and bibenzyl ether (BE), was investigated. Mg 2 Si was well distributed on the surface and in the voids of γ-Al 2 O 3 support. The Mg 2 Si/γ-Al 2 O 3 catalyst had high specific surface area, large amount of mesopores, strong basicity, and exhibited high catalytic efficiency in hydrocracking of 1-MON and BE due to the synergic effect between Mg 2 Si and γ-Al 2 O 3 . Under an initial hydrogen pressure of 3 MPa and reaction time of 60 min, the conversion of 1-MON and BE reached 100% when the reaction temperatures were 225 and 175°C, respectively. The selectivities for naphthalene and toluene were close to 100%, only traces of the hydrogenated products were detected. After 4 cycle tests, the catalytic activity of Mg 2 Si/γ-Al 2 O 3 catalystdropped to 50%.
研究领域:
化学工程
·
催化材料
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Peibo Li,Guoqiang Luo,Guinan Zhao,Huawu Liu,Yi Sun,Qiang Shen
Al powder is prone to oxidation, which can introduce impurities in powder metallurgy. In this study, Al 2 O 3 nanonetworks were obtained by destroying the oxide layer through Paulse Activated Sintering (PAS). The network and the nano-precipitation enhance the mechanical properties of Al-Cu-O composites. TEM analysis revealed the formation of CuAl 2 and an Al 2 O 3 network at the grain boundaries. The current facilitated the modulation of the intermetallic compound size and the fragmentation of the oxide layer. The current-induced discharge at the particle interfaces generated localized heating. Higher temperature effectively disrupts the oxide layer. The Al 2 O 3 network improved the fracture toughness of the Al-Cu-O composites by passivating crack propagation. Simultaneously, the current reduced the nucleation barrier for precipitation by promoting directional atomic migration. Uniformly dispersed nano-precipitates are conducive to the improvement of strength. This study provides new insights into oxidation-related challenges in Al powder.
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产品关联
DOI
高影响因子
Anti-Cancer Agents in Medicinal Chemistry
·
2018
·Vol. 18
·期 11
·1639-1648
·
IF 2.556
Xiao Daipeng,He Fen,Peng Dongming,Zou Min,Peng Junying,Liu Pan,Liu Yanfei,Liu Zhenbao
Background: Berberine (BBR), an isoquinoline plant alkaloid isolated from plants such as Coptis chinensis and Hydrastis canadensis, own multiple pharmacological activities. Objective: In this study, seven BBR derivatives were synthesized and their anticancer activity against HeLa
cervical and A549 human lung cancer cell lines were evaluated in vitro. Methods: The anti-cancer activity was measured by MTT assay, and apoptosis was demonstrated by the annexin V-FITC/PI staining assay. The intracellular oxidative stress was investigated through DCFH-DA assay. The molecular
docking study was carried out in molecular operating environment (MOE). Results: Compound B3 and B5 showed enhanced anti-cancer activity compared with BBR, the IC50 for compound B3 and B5 were significantly lower than BBR, and compound B3 at the concentration of 64 or 128 μM induced
apoptosis in HeLa and A549 cell lines. The reactive oxygen species (ROS) was generated in both cell lines when treated with 100 μM of all the compounds, and compound B3 and B5 induced higher activity in the generation of ROS, while compound B3 exhibited the highest activity, these results
are in accordance with the cytotoxicity results, indicating the cytotoxicity were mostly generated from the oxidative stress. In addition, molecular docking analysis showed that compound B3 had the greatest affinity with Hsp90. Upon binding, the protective function of Hsp90 was lost, which
might explain its higher cytotoxicity from molecular interaction aspect. Conclusion: All the results demonstrated that compound B3 and B5 showed significantly higher anti-cancer ability than BBR, and compound B3 is a promising anticancer drug candidate.
研究领域:
药理学
·
肿瘤学
·
化学
·
分子生物学
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DOI
PubMed
高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Guozhen Fang,Dantong Zhang,Xinyu Tong,Minghua Xu,Chunsheng Ding,Depeng Meng,Haiyan Zhang,Jing Leng,Dian Zhang,Lei Zhang,Kun Qi,Xiaowen Ruan,Xiaoqiang Cui
Amorphous cocatalysts effectively enhance the photoelectrochemical (PEC) water oxidation performance of BiVO4 (BVO). Nonetheless, their ability to extract photogenerated holes still suffers from limited efficiency and directionality. Here, we deliberately fabricate Ru single atoms immobilized on amorphous NiFeAl layered double hydroxide (NiFeAl-a) cocatalysts as a hole transport mediator and systematically elucidate the underlying promotion mechanism. Our investigations reveal that the formation of Ru−O hybridization states near the Fermi level augments the energy difference between BVO and NiFeAl-a. This modulation increases the band bending at their heterointerface, thereby facilitating hole extraction and suppressing the backflow of photogenerated electrons. These synergistic effects promote spatial charge separation. As a result, BVO/NiFeAl-a/Ru achieves a photocurrent density of 6.78 mA/cm2 at 1.23 V versus the reversible hydrogen electrode (vs RHE) and a half-cell applied bias photon-to-current efficiency of 2.63% at 0.61 V vs RHE. These values are higher than those of BVO/NiFeAl-a, which are 5.77 mA/cm2 and 2.20%, respectively. This work provides insights into the development of PEC systems for water oxidation.
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MACROMOLECULES
·
2026
·
IF 5.2
Mingsheng Liu,Lian He,Shuanjin Wang,Dongmei Han,Sheng Huang,Min Xiao,Yuezhong Meng
Polythiocarbonates (PTCs) represent a class of polymers derived from polycarbonates. While numerous synthetic methodologies have been reported, their practical applications remain unexplored. This study employs a one-pot bulk polymerization approach using propylene oxide (PO) and carbon disulfide (CS2) to synthesize polythiocarbonates, systematically investigating the effects of reaction temperature and duration on polymer properties. Results demonstrate that optimized reaction conditions fail to suppress O/S exchange, inevitably yielding polymers containing diverse thiocarbonate groups with varying stabilities. Consequently, we established the structural thermal stability hierarchy of thiocarbonate linkages: S(C═O)O > S(C═O)S > O(C═S)O > S(C═S)S > S(C═S)O. Density functional theory (DFT) calculations of bond dissociation energies (BDEs) corroborate this experimentally determined sequence. Our findings identify inherent structural instability as the fundamental barrier to polythiocarbonate applications, providing critical design principles for developing functionally stable PTCs.
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产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Qingqing Zhang,Cong Liu,Chang Xu,Dingnan Huang,Cheng Xie,Zhandong Wang,Xiao-Ming Cao,Jinlong Zhang,Juying Lei,Ziwei Ye,Lingzhi Wang
Upgrading light alkanes to value-added olefins is a long-standing challenge, owing to the high stability of C–H bonds and the tendency for overoxidation at elevated temperatures. Here, we introduce a light-driven strategy for ethane dehydrogenation using Cu-doped TiO 2 , in which atomically dispersed Cu coordinated to bridging oxygen (O br–Cu ) creates well-defined [Cu–O] ensembles that orchestrate site-specific, stepwise C–H activation. Photogenerated holes localize at O br–Cu sites to initiate the first C–H cleavage, while adjacent Cu centers mediate β–H elimination and H 2 evolution. In contrast, minor β–H activation at O br–Ti sites generates *H species that cannot desorb due to a prohibitive coupling barrier with *H on O br–Cu , leading to Cu reduction and progressive deactivation. Co-feeding CO 2 restores the active Cu coordination environment and suppresses this deactivation process without perturbing the primary reaction pathway. This cooperative design achieves a C 2 H 4 production rate of 21.1 mmol g −1 h −1 with nearly stoichiometric H 2 evolution and an apparent quantum efficiency of 6.1% under 365 nm irradiation. These findings establish a site-defined, hydrogen-conserving route for photocatalytic alkane upgrading, offering a general blueprint for selective C–H bond transformations with long-term stability. Converting light alkanes into useful olefins is hard because strong bonds and heat drive overoxidation. This study uses a copper-doped titanium dioxide photocatalyst to steer bond breaking, yielding ethylene and hydrogen.
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PubMed
高影响因子
ACS Omega
·
2026
·
IF 5.2
Zhi Qiao,Xiaona Yang,Jiaozhuang Liu,Liangting Liu,Xiaoxiao Meng,Xianying He,Gang Liu,Yan-Bin Teng,Qi Chen
O-Methylation represents a prevalent tailoring modification in natural product biosynthesis, significantly altering molecular properties and bioactivity. In this study, we report the crystal structure of the O-methyltransferase (MTase) McbD in complex with S-adenosyl-l-homocysteine (SAH) at 3.0 Å resolution, complemented by a modeled binding pose for the substrate marinacarboline B (1). Through integrated site-directed mutagenesis and enzymatic assays, we identified critical residues required for catalytic activity and propose a refined mechanistic model for methyl transfer. These findings offer substantive structural and mechanistic insights into how O-MTases drive the diversification of bioactive natural products.
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DOI
PubMed
高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Baixin Lin,Siyuan Li,Dashan Zhang,Junbo Wang,Peiyu Liu,Yang Shi,Xiaoqing Zheng,Yongkang Huang,Lintai Da,Sibao Wang,Zixin Deng,Delin You,Lingxin Kong
Enzyme engineering provides a powerful route to diversify the chemical space of complex natural products for drug discovery. Here, we reprogram the ribosome-targeting antibiotic anisomycin through the engineering of its late-stage O-methyltransferase AniK. By integrating structure-guided rational design with artificial intelligence (AI)-assisted computational screening, we generated AniK variants with expanded cofactor promiscuity, enabling the transfer of diverse alkyl groups from noncanonical S-adenosylmethionine analogues. Concurrently, a structure-based generative algorithm (DELETE) was employed to design a focused library of phenolic hydroxyl modified anisomycin derivatives, which were synthesized via a one-pot enzymatic cascade using the engineered halide methyltransferase AclHMT-v16 and the optimized AniK mutant M144A-A133D. This integrated platform delivered 14 structurally diverse anisomycin derivatives, among which compounds 7 and 15 exhibited enhanced antidermatophyte activity while maintaining potent ribosome targeting capability. Our work establishes a reprogrammable enzymatic platform for the late-stage diversification of anisomycin, providing a modular strategy to access bioactive analogues with optimized therapeutic potential.
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