APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Xiaoshun Wei,Xuechun Yang,Yun Guo,Yinzhong Liu,Lingchao Wang,Qingjie Wang,Lingli Cheng,Zheng Jiao
In this study, a novel UV-enhanced Mg-doped MOF-ZnO sensor was investigated for its efficient detection of n-butanol gas at lower temperatures. The composite samples were prepared by the co-precipitation method with the appropriate component ratio. The structure, morphology, and optical properties of the as-prepared samples were systematically analyzed through XRD, SEM, TEM, BET, XPS, and UV–vis characterizations. The gas-sensitive performances based on the pristine MOF-ZnO and Mg-doped MOF-ZnO sensor series with the doping levels of 1 %, 3 %, 5 %, and 7 % (wt%) were comprehensively evaluated by adopting the gas-sensitive system. Among them, the 3 % Mg:MOF-ZnO sensor has given prominence to the largest specific surface area and highest oxygen vacancy concentration demonstrating the most excellent gas-sensing performance. Furthermore, with the aid of UV excitation, the 3 % Mg:MOF-ZnO sensor had achieved the enhanced response value of 2049 that was 4.44 times higher than that of pristine MOF-ZnO to 100 of ppm n-butanol at a low temperature of 246 °C, additionally presented out the superior reproducibility with speedy response/recovery time (12/22 s), the theoretical detection limit as low as 200 ppb, as well as the excellent long-term stability and selectivity for n-butanol. This study offers a promising strategy for the well-development of high-performance n-butanol sensors.
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CHINESE JOURNAL OF CHEMISTRY
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2024
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IF 5.5
Dongxiao Wang,Zheng Lan,Yue Li,Ying Huang,Kun Yin,Lixia Yang,Liangjiu Bai,Donglei Wei,Huawei Yang,Hou Chen,Mingchuan Luo
Comprehensive Summary Photocatalytic aerobic oxidative desulfurization (PAODS) is a sustainable alternative technology to traditional, energy-intensive fuel desulfurization methods. Nonetheless, its advancement is hindered by the notable challenge of inadequate electron-hole separation efficiency within the existing catalytic systems. Herein, a Janus 2D/2D heterostructure composed of Co 3 O 4 and CoMoO 4 is reported for the PAODS of thiophenic sulfides. Through a combination of detailed experimental characterizations and density functional theory (DFT) calculations, we elucidate the formation of a type II p-n heterojunction in the catalyst, significantly enhancing electron-hole separation through electric field force and reducing the possibility of electron-hole recombination due to the spatial separation of redox centres. The photocatalyst exhibits exceptional activity and demonstrates an impressive performance of 10.4 mmol·g –1 ·h –1 in the oxidation of dibenzothiophene (DBT). Moreover, the photocatalyst demonstrates profound desulfurization capabilities in real diesel, reinforcing its promising prospects for industrial application. These discoveries provide invaluable insights, both scientifically and practically, towards the development of advanced photocatalysts for PAODS processes.
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Molecular Catalysis
·
2025
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IF 4.9
Bo Jiang,Shu-Lin Liu,Zhe-Yan Jin,Zhao Wang,Bin-Can Cheng,Ze-Long Guan,Ying Hong,Zhao Wei,Zhi Qiao,Jian Tao,Bao-Lian Su
Selective hydrogenation driven by heat is a critical industrial process for purifying alkene feedstocks with serious problems of energy and H 2 consumption. Photochemistry-assisted strategy offers a sustainable alternative owing to its superiority of H 2 -free reaction under ambient temperature, unfortunately, with a challenging demand on efficient catalysts. Herein, a wide-spectrum-responsive Pd/N-TiO 2 photo-thermal catalyst was developed by a solvothermal method for photochemistry-assisted selective hydrogenation of butadiene in propene. It shows an excellent catalytic performance, with 100 % alkenes selectivity and 100 % butadiene conversion under irradiation of full-light (i.e., 320 nm∼780 nm). Notably, over 53 % butadiene conversion with 100 % alkenes selectivity was successfully retained on Pd/N-TiO 2 after shortening the wavelength range to visible light, much superior to that on Pd-TiO 2 (i.e., <1 % butadiene conversion). Further exploration reveals that the nitrogen doping extends the light-responsive wavelength of titanium oxide from ∼380 nm to above 500 nm owing to the formation of Ti 3+ and oxygen vacancies, which later create a defect energy level (i.e., ∼-0.53 to -0.12 eV) between the valence-conduction band of TiO 2 . The wide spectral response of N-TiO 2 enhances the water photolysis to produce intermediate hydrogen ([H]) that acts as the hydrogen source for the tandem butadiene hydrogenation over the Pd surface. The work indicates that developing a dual-functional catalyst with an expanded light-responsive wavelength is an efficient way to enhance the photochemistry-assisted selective hydrogenation.
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ACS Catalysis
·
2025
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IF 13.1
Qianqian Song,Yingbing Zhang,Ziyang Wu,Min Kuang,Jun Chen,Jianping Yang
The electrocatalytic urea synthesis has emerged as a promising alternative strategy to replace the current energy-intensive industrial Haber–Bosch processes which are limited by sluggish C–N coupling and low selectivity because of the unmatched reduction kinetics of CO2 and nitrogen-based precursors. Herein, a thermodynamically spontaneous early stage C–N coupling pathway of *CO2 + *NO → *NOCO2 is established through the asymmetric bridging-adsorption of CO2 enabled by hydroxycarbonate-induced CO32–-Cu2+ dual sites on the tandem electrocatalyst of copper carbonate hydroxide and iron oxide grown on carbon fibers (CuCH/α-Fe2O3–CFs). This asymmetric adsorption induces a pronounced electron-deficient state of carbon atoms in CO2 due to bidirectional electron transfer toward both the CO32– and the Cu2+ centers. Coupled with the directional migration of *NO intermediates at the interface, effectively suppress the subsequent protonation of *CO2 while promoting nucleophilic attack by *NO, thereby driving spontaneous initial C–N coupling of *CO2 and *NO and significantly lowering the energy barrier of the C–N coupling step. The results demonstrate a urea Faradaic efficiency of 78.7% and urea yield rate of 1794.6 μg h–1 mgcat–1 at an ultralow applied potential of −0.20 V vs RHE, surpassing most reported catalysts to date.
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ADVANCED MATERIALS
·
2024
·Vol. 36
·期 18
·2309844
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IF 27.4
Rundong Fan,Wei Sun,Congmeng Li,Yihua Chen,Haipeng Xie,Yongli Gao,Yue Ma,Zongyang Peng,Zijian Huang,Ruiyang Yin,Fengtao Pei,Wentao Zhou,Yuetong Wu,Huifen Liu,Kailin Li,Tinglu Song,Dechun Zou,Huachao Zai,Hui Li,Qi Chen,Qian Wang,Huanping Zhou
Metal halide perovskite solar cells (PSCs) have garnered much attention in recent years. Despite the remarkable advancements in PSCs utilizing traditional metal electrodes, challenges such as stability concerns and elevated costs have necessitated the exploration of innovative electrode designs to facilitate industrial commercialization. Herein, a physically and chemically stable molybdenum (Mo) electrode is developed to fundamentally tackle the instability factors introduced by electrodes. The combined spatially resolved element analyses and theoretical study demonstrate the high diffusion barrier of Mo ions within the device. Structural and morphology characterization also reveals the negligible plastic deformation and halide-metal reaction during aging when Mo is in contact with perovskite (PVSK). The electrode/underlayer junction is further stabilized by a thin seed layer of titanium (Ti) to improve Mo film's uniformity and adhesion. Based on a corresponding p–i–n PSCs (ITO/PTAA/PVSK/C 60 /SnO 2 /ITO/Ti/Mo), the champion sample could deliver an efficiency of 22.25%, which is among the highest value for PSCs based on Mo electrodes. Meanwhile, the device shows negligible performance decay after 2000 h operation, and retains 91% of the initial value after 1300 h at 50–60 °C. In summary, the multilayer Mo electrode opens an effective avenue to all-round stable electrode design in high-performance PSCs.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Lingxiao Xue,Jiahao Cui,Ruiying Li,Wenhe Xie,Keyu Chen,Hongxiu Yu,Limin Wu,Tianjun Ni,Qin Yue,Yonghui Deng
Cells have greatly inspired advancements in chemical processes, including leveraging the idea of cascade catalysis to drive thermodynamically unfavorable reactions and mimicking the compartmentalized architecture to design novel nanostructures. Here, a single-particle cascade catalysis promoted gas sensing platform is inspired to be designed (denoted as CoSnO 3 @mCeO 2 ) by positionally assembling n-type mesoporous CeO 2 catalytic shell on p-type CoSnO 3 gas sensitive core. Uniform CoSn(OH) 6 @mCe(OH) x core–shell particles with tailored mesostructures, tunable large mesopores, and adjustable shell thicknesses are first constructed. After thermal treatment, CoSnO 3 @mCeO 2 particles are obtained, which serve as cascade catalysis enhanced sensitive layer for fabricating gas sensors with independent catalytic and sensing control. As a proof-of-concept, the CoSnO 3 @mCeO 2 gas sensors exhibit nearly three times higher acetone sensitivity ( R g /R a = 26.81–50 ppm) than individual CoSnO 3 sensors with an ultralow limit of detection of 5.22 ppb. The enhanced sensitivity is achieved through a tandem catalytic reforming-oxidation sensing procedure, which begins with the primary catalytic reforming of acetone to acetic acid in the mCeO 2 shell, followed by the secondary sensing reaction of acetic acid in the CoSnO 3 core. The design concept of cascade catalysis promotes gas sensor can serve as a paradigm for developing single-particle functional nanodevices for various applications.
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Advanced Energy Materials
·
2019
·Vol. 9
·期 22
·1900149
·
IF 24.884
Jiabin Wu,He Zhou,Qun Li,Ming Chen,Jun Wan,Nian Zhang,Liukang Xiong,Song Li,Bao Yu Xia,Guang Feng,Meilin Liu,Liang Huang
Atomically dispersed transition metals confined with nitrogen on a carbon support has demonstrated great electrocatalytic performance, but an extremely low concentration of metal atoms (usually below 1.5%) is necessary to avoid aggregation through sintering which limits mass activity. Here, a salt-template method to fabricate densely populated, monodispersed cobalt atoms on a nitrogen-doped graphene-like carbon support is reported, and achieving a dramatically higher site fraction of Co atoms (≈15.3%) in the catalyst and demonstrating excellent electrocatalytic activity for both the oxygen reduction reaction and oxygen evolution reaction. The atomic dispersion and high site fraction of Co provide a large electrochemically active surface area of ≈105.6 m 2 g −1 , leading to very high mass activity for ORR (≈12.164 A mg Co −1 at 0.8 V vs reversible hydrogen electrode), almost 10.5 times higher than that of the state-of-the-art benchmark Pt/C catalyst (1.156 A mg Pt −1 under similar conditions). It also demonstrates an outstanding mass activity for OER (0.278 A mg Co −1 ). The Zn-air battery based on this bifunctional catalyst exhibits high energy density of 945 Wh kg Zn −1 as well as remarkable stability. In addition, both density functional theory based simulations and experimental measurements suggest that the Co N 4 sites on the carbon matrix are the most active sites for the bifunctional oxygen electrocatalytic activity.
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Reaction Chemistry & Engineering
·
2025
·
IF 3.1
Xiangyu Wen,Qiusheng Yang,Ming Li,Xiaoshu Ding,Peng Zhai,Yao Lu,Xinqiang Zhao,Yanji Wang,Dongsheng Zhang
Amino-methyl-N-phenylcarbamate (TMC) is an important organic intermediate. In this study, a new two-step route, i.e., methoxycarbonylation and direct amination reaction, was designed for synthesis of TMC. During this process, p-Toluidine first reacted with dimethyl carbonate to form metholylcarbamate (MTCM), and then MTCM further converted to TMC via direct amination reaction. It was found that in methoxycarbonylation process, Zn(OAc)2 catalyst was a better choice and p-Toluidine was almost completely converted into MTCM, corresponding to 99% p-Toluidine conversion and 95.4% MTCM yield. As for direct amination reaction, Fe-V/ZSM-5 bimetallic catalyst was selected and high yield of total TMC was obtained at 69.6%. The catalyst characterization results showed that the synthesized bimetallic catalysts retained the structural features of ZSM-5, while the abundance of metal ions on the surface promoted the reaction
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Advanced Energy Materials
·
2025
·
IF 26
Yao Wang,Jianrui Wang,Xiao Xu,Yan Wang,Baohai Jia,Shangyang Li,Kornelius Nielsch,Jiaqing He
The excellent performance of skutterudites is related to the interrelated filling fraction and doping limitation of the intricate matrix. Especially for the investigation of n-type electronegatively filling samples, the exceptionally low doping capacity at Sb sites leads to severely compromised thermoelectric performance. Here, a breakthrough is achieved in surpassing conventional doping limits by developing a novel “electrical compensation-bonding modulation” method, contributing to the reconfiguration of the unique X 4 ring structure (Consists of Sb 4 units) in S 0.2 Se 0.05 Co 4 Sb 12-x Te x skutterudites. The modulated bond hierarchy and disorder enable a concurrent regulation of phonon and carrier transport, resulting in a significant improvement of the transport properties. Building upon this foundation, a revolutionary off-center state has been introduced to the matrix via continuous doping of Se at Sb sites, aimed at suppressing the lattice thermal conductivity. Ultimately, a peak zT of 1.8 at 800 K is achieved, with an average zT of 1.1 across the 300–800 K temperature range. This work provides a universal approach to overcome doping limits in Co 4 Sb 12 -based thermoelectrics.
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ACS Applied Bio Materials
·
2025
·
IF 4.7
Xiaobing Ma,Xiangbin Sun,Rongmin Wang,Xiaoyu Han,Yuanyuan Xie,Yufeng He,Pengfei Song
Bacterial infection of surface-damaged fruit is one of the troubling issues in daily life. To address this issue, the β-cyclodextrin (CD) grafting N+-borneol ester antibacterial polymer (CD-NBOx), containing borneol with active groups and quaternary ammonium compounds (QACs) positive charges, was successfully synthesized using RAFT and characterized by NMR, Fourier-transform infrared, and gel permeation chromatography. Its antibacterial activity and biofilm inhibition were evaluated against Escherichia coli and Staphylococcus aureus, and the adhesion resistance was measured by crystal violet (CV) staining experiments. It indicated that the antibacterial rate of CD-NBOx reached 99.9 and 87.3% and the biofilm inhibition rates were up to 97.5% against E. coli. Interesting, there was no spoilage of the fruit and only 20% weight loss in the 15-day fruit preservation experiment. CD-NBOx possesses excellent antibacterial and adhesion resistance due to the synergy between cyclodextrin for biocompatibility and N cation for antibacterial and borneol stereochemistry. In summary, CD-NBOx as a constructing “offensive and defensive integrated” is validated as a viable antibacterial material while also expanding potential life applications of N+-borneol ester polymers in fruit preservation in the future.
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
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2025
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IF 4.9
Qingfeng Luo,Yuyi Deng,Qiyuan Yang,Nanxin Zhao,Can Wang,Xingsheng Li
Osteopontin (OPN), highly expressed in foam cells, serves as a hallmark of atherosclerotic plaques and a potential target for site-specific drug delivery. In this study, we developed OPN-targeted liposomes (OPN LIP) co-loaded with curcumin and perfluoro-n-pentane (PFP) to enhance therapeutic efficacy against atherosclerosis. The liposomes exhibited uniform particle size, colloidal stability, favorable biocompatibility, and minimal cytotoxicity. In vitro experiments demonstrated efficient and time-dependent cellular uptake by ox-LDL–stimulated RAW264.7 foam cells. Upon exposure to low-intensity focused ultrasound (LIFU), the nanocarriers underwent acoustic cavitation-induced rupture, leading to rapid curcumin release and significant induction of apoptosis. OPN LIP treatment notably reduced IL-1α and TNF-α levels and aggravated apoptosis in foam cells. Transcriptomic analysis revealed modulation of inflammatory and apoptotic pathways, including TLR, NF-κB, and Mapk3 signaling. These findings highlight the potential of OPN LIP as an ultrasound-responsive, targeted nanoplatform capable of suppressing inflammation and foam cell viability, providing a promising approach for the treatment of atherosclerosis through combined physical and pharmacological strategies.
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CLINICAL RHEUMATOLOGY
·
2025
·
IF 2.8
Yin Jia,Yin Xuan,Tao Lei,Peng Yuanzhi,Zhao Shuhan,Hou Haifeng,Yin Xinyue,Ran Zhangshen,Zhou Aihong,Ding Guoyong
Background Alterations in immunoglobulin G (IgG) N -glycosylation have been implicated in various diseases, potentially including ankylosing spondylitis (AS). However, empirical evidence regarding the associations IgG N -glycosylation, inflammatory factors, and AS is sparse. We aimed to investigate these associations and evaluate the diagnostic performance of IgG glycosylation traits as a biomarker for AS. Methods This case–control study recruited 142 AS patients and 142 controls. We used hydrophilic interaction liquid chromatography with ultra-performance liquid chromatography to detect the profiles of plasma IgG N -glycans. An enzyme-linked immunosorbent assay kit was used to measure the levels of serum inflammatory factors. We used multivariate logistic regression, canonical correlation analysis (CCA), and Lasso regression to analyze the data. Results Multivariate logistic analysis identified 14 IgG N -glycan-derived traits significantly associated with AS. The changes were primarily characterized by decreased galactosylation, sialylation, bisgalactosylated fucosylation and sialated fucosylation, alongside increased core fucosylation, agalactosylated fucosylation, neutral fucosylation and sialated bisecting N -acetylglucosamine. Significant differences were observed between cases and controls in levels of C-reactive protein (CRP), IL-17, IL-22, IL-6, and TNF-α. CCA demonstrated a moderate correlation between IgG N -glycan-derived traits and inflammatory factors ( r = 0.476). The combined diagnostic performance of derived traits and inflammatory factors yielded a higher area under the curve (AUC = 0.90) than either alone (AUC derived traits = 0.88, AUC inflammatory factors = 0.78). Conclusion The findings indicate that abnormal IgG N -glycosylation may play an important role in the development of AS through promoting the pro-inflammatory function. The derived traits combined with inflammatory factors may serve as potential biomarkers to distinguish AS.
Key Points • We comprehensively analyzed IgG N-glycan-derived traits in AS by an HILIC-UPLC-based high-throughput method. • Abnormal IgG N-glycosylation plays a role in the development of AS through promoting the proinflammatory. • IgG N-glycosylation combined with inflammatory factors demonstrated strong diagnostic performance for AS.
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