JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Meichun Qin,Shiying Fan,Xinyong Li,Moses O. Tade,Shaomin Liu
Electroreductive C O coupling provides a prospective strategy for biomass derivative upgrading via reducing the number of oxygen-containing functional groups and increasing their molecular weight. However, exploring superior electrocatalysts with effective reactivity and high selectivity for target products are still a challenge. In this work, single atom Au surface derived NiMn 2 O 4 (SACs Au−NiMn 2 O 4 ) spinel synergetic composites were fabricated by a versatile adsorption-deposition method and applied in electroreductive self-coupling of benzaldehyde to dibenzyl ether . The SACs Au–NiMn 2 O 4 spinel synergetic composites enhanced electroreductive coupling of benzaldehyde, significantly improved the yield and selectivity of dibenzyl ether. Systematic characterizations and density functional theory calculation revealed that atomically dispersed Au occupied surface Ni 2+ vacancies, which played a dominated role in C O coupling of benzaldehyde. Detailed calculation results showed that benzaldehyde preferred to adsorb on Ni octa-hedral sites of NiMn 2 O 4 spinel synergetic structure, single atom Au surficial derivation over NiMn 2 O 4 further reduced the adsorption energy (E ads ) of benzaldehyde on SACs Au−NiMn 2 O 4 , thus the C O coupling of benzaldehyde to dibenzyl ether was promoted. Moreover, single atom Au surficial derivation lowered the energy barrier of rate-determining step, facilitated the formation of dibenzyl ether species. Our work also paves an avenue for rational design single atom materials using spinel as support.
研究领域:
化学
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材料科学
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PubMed
高影响因子
FUEL
·
2016
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IF 3.611
Mei-Xia Zhao,Xian-Yong Wei,Meng Qu,Jiao Kong,Zhan-Ku Li,Jing Liu,Zhi-Min Zong
A novel solid acid was prepared by impregnating trifluoromethanesulfonic acid (TFMSA) onto mesoporous ZrO 2 coated attapulgite (MPZCA) via one-pot synthesis method. Dibenzyl ether (DBE) was used as a coal-related model compound to evaluate the catalytic activity of TFMSA/MPZCA for cleaving C alk –O bridged bonds in low-rank coals. The results show that DBE conversion over TFMSA/MPZCA could reach 100% at 160 °C in C 2 H 5 OH without charging H 2 . TFMSA/MPZCA proved to be stable after 4 cycles with only slight loss in catalytic activity. Moreover, a H + transfer mechanism was proposed, which reasonably deduces possible pathways for DBE hydrocracking over TFMSA/MPZCA.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
FUEL
·
2023
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IF 7.4
Jiale Gu,Huan Li,Wencai Peng,Di Zhu,Jiajia Chen,Shengjie Luo,Siming Liu,Wenxiang Zhao,Youqing Wu,Sheng Huang,Shiyong Wu
The hydrogenation properties of dibenzyl ether (an oxygenated model compound of lignite) via the water–gas shift reaction (WGSR) were studied in a subcritical CO-H 2 O system. The result showed during the hydrogenation process, the C-O bond was broken, and the fragments of dibenzyl ether were stabilized by the hydrogen generated by WGSR, generating benzene, toluene, benzyl alcohol and benzaldehyde. The presence of excess water inhibited the hydrogen transfer, largely reducing the conversion of dibenzyl ether. However, the inhibition effect was substantially reduced when the reaction environment reached the critical temperature and subcritical pressure of water. The hydrogen and deuterium generated by H 2 O and D 2 O via WGSR were utilized to label and analyze the hydrogenation position of the product, respectively. The results showed that the hydrogen generated by WGSR was added to the methylene after the break of dibenzyl ether, and this hydrogen appeared on the benzene ring structure via hydrogen transfer. The bond dissociation energy and energy required for the hydrogenation process of dibenzyl ether under aqueous condition were calculated by utilizing density functional theory (DFT). First, hydrides (H − ) are formed by the WGSR under alkaline conditions. Then, the formation energy (140.81 kJ/mol) of hydrides and the energy (15.54 kJ/mol) of hydrides attacking the dibenzyl ether to form the transition state were lower than the bond dissociation energy (259.26 kJ/mol) of the dibenzyl ether. That is, the hydrogenation of dibenzyl ether via WGSR prefers to be a nucleophilic reaction rather than a pyrolysis reaction. In the coal liquefaction process, the hydrides produced by WGSR under the catalysis of alkali is conducive to the hydrocracking of oxygen containing functional groups.
研究领域:
化学工程
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能源科学
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催化反应
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DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2021
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IF 6.186
Hao Xu,Xing Fan,Guo-Sheng Li,Yang-Yang Xu,Wen-Long Mo,Peter N. Kuznetsov,Feng-Yun Ma,Xian-Yong Wei
Co-Mo/γ-Al 2 O 3 bimetallic catalyst was prepared by incipient wetness impregnation and the physicochemical properties were obtained by a series of characterization methods. The active components are mainly MoS 2 and Co-Mo-S existing on γ-Al 2 O 3 , the support. Meanwhile, the activity of catalyst in hydroconversion of four coal-related model compounds (CRMCs), dibenzyl ether, furan, thiophene and quinoline, was investigated. Hydroconversion products were analyzed by gas chromatography/mass spectrometry (GC/MS) and the possible reaction pathways were proposed according to the GC/MS data. Oxygen was removed from dibenzyl ether via the direct cleavage of C alk -O bridge bond to produce benzylium cation followed by the combination with H − to generate toluene. The hydroconversion of furan can be realized by the direct cleavage of C ar -O bond and direct hydrogenation, respectively. For thiophene, H + directly transferred to sulfur atom, leading to the cleavage of C ar -S bond to produce H 2 S and 1,3-butadiene, which abstracted active hydrogen to yield butane. Another indirect desulfurization pathway for thiophene is hydrogenating to form tetrahydrothiophene and C–S bond cracking to produce butane. Hydroconversion of quinoline started with either N-ring or benzene ring , and the first one was the main pathway.
研究领域:
催化化学
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煤炭化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Xue Xing,Fuyun Yang,Yuying Yang,Guodong Yang,Xiao Xiao,Hongyu Chen,Xueyang Liu
In the field of ionic-liquid-based electrochemical gas sensors, the high viscosity of ionic liquids leads to slow mass transfer, restricting sensor performance. In this study, microstirbars with tunable sizes were fabricated via wet spinning. Using fluorescent dye as a tracer, these microstirbars homogeneously dispersed the dye in a droplet of ionic liquid within 2 min, nearly 200 times faster than the control group without stirring. When using ferrocene as a model reactant in chronoamperometry, the microstirbars enhanced the mass transfer process and the best stirring conditions (400 rpm, 8.0 wt %, l = 300 μm) were determined. When these optimized conditions were applied to oxygen detection, the results showed that the sensor sensitivity reached 0.63 μA·%–1, on par with the best performing gas sensors in the literature and 6 times higher than the control group without stirring. The stirred sensor achieved T90 of 7.0 s for 6.7% O2, three times faster than that of the control group without stirring (21 s). This study presents a straightforward approach to addressing the mass transfer challenges in ionic liquids, serving as a viable alternative to the complex designs of electrochemical sensors. As an approach to enhance mass transfer in microdroplets, we believe that the microstirring strategy is not limited to gas sensors. With advances in miniaturization of electromagnetic devices, it holds promise for a variety of sensing schemes.
研究领域:
电化学
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传感器与传感技术
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微流控
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材料科学
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分析化学
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PubMed
高影响因子
Reaction Chemistry & Engineering
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2025
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IF 3.1
Xinlei Jia,Yonghui Wang,Dezhong Wang,Yingying Hu,Lanjuan Xu,Qing Cao,Chao Liu,Lixin Wei
Crude oil emulsions are challenging to break due to their complex and variable composition. While high-performance demulsifiers exist, many conventional systems still face limitations such as poor stability under harsh conditions or insufficient separation efficiency for specific emulsion types. It is thus essential to develop new demulsifiers that combine high salt resistance with effective destabilization capability. Carbon materials, known for their strong adsorption capacity and chemical stability, can efficiently capture emulsified droplets, enabling significantly enhanced demulsification performance even under harsh conditions. The integration of TiO2–carbon heterostructures with fluorinated polyether grafting into magnetic demulsifiers represents a previously unreported strategy. Building on this background, our research innovatively modified the magnetic substrate Fe3O4 by incorporating TiO2 and three types of carbon materials (carbon nanospheres, graphene oxide, and carbon nanotubes). Through a sol–gel approach, fluorinated polyether chains were covalently grafted onto the surface of modified Fe3O4 nanoparticles, leading to the successful synthesis of three novel magnetic composite demulsifiers: Fe3O4@Ti/C–F, Fe3O4@Ti/G–F and Fe3O4@Ti/CN–F. The results demonstrate that these three demulsifiers exhibit excellent demulsification efficiency, acid resistance, and excellent recyclability. They achieve demulsification rates exceeding 85% in neutral and acidic environments. Notably, Fe3O4@Ti/G–F stands out with the best performance. After five cycles of recovery from a biphasic system, its demulsification efficiency remains above 70%. When used at a concentration of 600 mg L−1, it can achieve a demulsification rate of 93.44% within just 30 minutes. In summary, this innovative magnetic nanodemulsifier not only provides an efficient and stable solution for crude oil emulsion separation but also offers significant ecological benefits, holding great potential for application in the treatment of oily wastewater.
研究领域:
环境科学与技术
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材料科学
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纳米技术
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石油工程
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水处理
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2026
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IF 8.5
Guangai Sun,Shijie Guo,Yuanyuan Yao,Zeyu Lin,Hui Gao,Roland H. Stauber,Bin-Chun Li,Guo-Bin Ding
α-L-Rhamnosidase is a significant biocatalyst that specifically cleaves terminal α-L-rhamnose group from natural flavonoid diglycosides, enabling the biocatalytic production of high-value flavonoid glucosides like prunin from naringin. Compared to its precursor naringin, prunin exhibits superior solubility and bioavailability, making this enzymatic conversion commercially valuable for the food and pharmaceutical industry. However, the industrial application of free α-L-rhamnosidases faces significant challenges, including enzyme instability, difficulty in recovery, and unsatisfactory reusability. To address these issues, this study developed an innovative magnetically recoverable biocatalyst (Fe₃O₄-Rha) through covalent immobilization of recombinant α-L-rhamnosidase from human fecal metagenome onto Fe₃O₄ nanoparticles using EDC/NHS chemistry, and the immobilization parameters were systematically optimized. The successful preparation of Fe₃O₄-Rha was verified by TEM, FTIR, TGA, and SQUID analysis. Fe₃O₄-Rha retained the catalytic property of free Rha in terms of optimal pH and temperature but exhibited superior tolerance on organic solvent especially ethanol and isopropanol. Moreover, Fe₃O₄-Rha could effectively biotransform naringin to prunin and maintained 61.34% of initial activity after 5 cycles. In a scaled-up reaction system, Fe₃O₄-Rha also efficiently converted naringin into prunin and the complete conversion was achieved within 10 h. This work successfully developed a magnetically recoverable immobilized α-L-rhamnosidase system for the efficient and reusable biotransformation of naringin, offering a promising approach for the enzymatic modification of bioactive small molecules using biological macromolecular catalysts.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
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2026
·Vol. 18
·期 31
·42780-42788
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IF 7.8
Zou Lie,Huang Xiao-Yan,Zhang Yi,A Yao-Lin,Xu Qing-Chi,Chen Bing-Hui,Liu Jinxuan,Zhang Hua,Li Jian-Feng
Understanding the molecular origins of oxygen reduction reaction (ORR) activity on Pt-based catalysts is essential for the rational design of high-performance electrocatalysts. Herein, by combining electrochemical measurements with in situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), we systematically investigate the ORR pathway on Pt-based alloy nanocatalysts incorporating different transition metals to elucidate how surface oxygenated intermediates dictate ORR activity. Among the catalysts examined, PtNi exhibited higher activity than PtFe, PtCo, and commercial Pt/C, underscoring the pronounced sensitivity of intrinsic ORR activity to alloy composition. Potential-dependent in situ Raman spectra, corroborated by isotopic labeling, directly identified *OOH as a key ORR intermediate and established a clear correlation between its vibrational frequency and catalytic activity. The results suggest that Ni alloying may modify the electronic environment of Pt, thereby weakening the Pt-O interaction, optimizing the adsorption state of the kinetically relevant *OOH intermediate, and consequently promoting ORR kinetics. This study establishes an effective spectroscopic platform for probing ORR intermediates on realistic electrocatalyst surfaces and offers molecular-level understanding of the activity enhancement in Pt-based alloy catalysts.
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PubMed
高影响因子
Advanced Science
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2026
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IF 14.1
Tao Shen,Hongdou Shen,Weiyue Wu,Zhuoying Jiang,Bin Liu,Yansi Xian,Rui Peng,An Yan,Yu Ben,Yong Shi,Xiang Chen,Baosheng Guo,Qing Jiang,Weijun Wang,Pingqiang Cai
The clinical intractability of diabetic foot ulcers stems from a profound uncoupling of cutaneous neurovascular networks, rendering standard metabolic and topical interventions largely palliative. Paradoxically, remote orthopedic trauma robustly accelerates distal skin repair, yet the systemic molecular mediators driving this “bone-skin crosstalk” remain undefined, precluding its translation into non-invasive therapies. Here, we establish that macroscopic bone fracture expedites diabetic wound healing through the systemic release of exosomal miR-130b-3p, a potent orchestrator of coupled angiogenesis and neurogenesis. To recapitulate this physiological axis non-invasively, we engineered a self-assembling, cholesterol-modified agomir-130b-3p nanocomplex that could bypass endolysosomal degradation. For sustained spatial delivery, these carrier-free nanoassemblies were incorporated into an in situ photocrosslinkable methacrylated collagen/silk fibroin hydrogel, creating a bio-instructive extracellular matrix that prolongs microRNA bioavailability. In streptozotocin-induced diabetic mice, hydrogel-mediated agomir delivery achieved 97.2% full-thickness wound closure. Advanced volumetric light-sheet imaging of chemically cleared whole-mount skin confirmed the robust spatiotemporal reconstruction of deep vascular and neural networks. These findings decode a distinct exosome-mediated inter-organ repair mechanism and demonstrate that biomimetic microRNA nanoformulations can effectively translate systemic physiological cues into localized, high-efficacy therapeutics for ischemic neuropathic wounds.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 5
·124698
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IF 7.5
Jing-jing Wu,Jia-yuan Tian,Feng Lin,Yu-long Ma,Yong-gang Sun,Pei Ma,Shuai-lei Li,Xue Zhang,Yi-shu Ma,Xiao-lin Xue
The efficient hydrodeoxygenation (HDO) of lignin oil to produce high-value-added cycloalkanes is a key route for biomass resource utilization. However, developing catalysts with both high catalytic activity and product selectivity remains a crucial challenge in this field. Herein, a strategy integrating crystalline-phase regulation and hydrogen spillover was proposed. Ru was doped into the ZIF-67 precursor via a one-pot method. After controlled calcination and hydrogen reduction, a nitrogen-doped carbon-coated Ru-Co bimetallic catalyst (RuCo@NC) was successfully prepared. Characterization results showed that the introduction of Ru induced the phase transformation of Co from face-centered cubic (FCC) to hexagonal close-packed (HCP) and precisely regulated the electron density distribution of catalytic active sites through Ru to Co electron transfer. H 2 -TPR/TPD confirmed that Ru, as a hydrogen spillover site, significantly enhanced low-temperature reducibility and hydrogen adsorption capacity. DFT calculations indicated that Ru sites dominated the efficient dissociation and activation of H₂ molecules, while Co sites were responsible for the selective adsorption of substrate molecules. The synergistic effect between the two metals greatly improved the HDO activity of the catalyst. The optimized 0.009RuCo@NC-400 catalyst achieved 100% conversion of lignin oil at 240 °C and 2 MPa H₂, with a cycloalkane selectivity of 73.7%. Moreover, the conversions of ten lignin derivatives were all above 97%. This study reveals a synergistic catalytic mechanism of the 0.009RuCo@NC-400 catalyst, integrating crystalline phase structure, electronic effects, and hydrogen spillover, providing theoretical guidance for the design of efficient HDO catalysts.
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高影响因子
Scientific Reports
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2026
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IF 4.9
Jiang Yumiao,Gu Xinyi,Deng Jin,Yin Xiaofeng
Sensory and sympathetic nerves contribute to skeletal homeostasis, bone repair, and pain transmission, but the segmental origins of neurons innervating individual limb bones remain unclear. Here, we combined multiplex retrograde fluorescent tracing with three-dimensional imaging of solvent-cleared organs (3DISCO) to map sensory and sympathetic neurons projecting to mouse limb bones. Tracer-positive dorsal root ganglia (DRG) and sympathetic ganglia (SG) neurons were quantified across spinal segments, and normalized distributions were analyzed using dominant segments, dominance index, Shannon entropy, and hierarchical clustering. Upper-limb bones mainly received lower cervical and upper thoracic inputs, whereas lower-limb bones were associated with lumbar inputs. Sensory neurons innervating the humerus, radius, femur, and tibia were distributed across C4-T1, C5-C8, L1-L6, and L1-L5 DRG, respectively. Sympathetic neurons showed more restricted distributions, with humerus, radius, femur, and tibia inputs concentrated in T1-T2, T1, L4-L5, and L4 SG, respectively. Exploratory integration with public bone transcriptomic datasets suggested candidate molecular signatures related to developmental patterning, metabolic/cytoskeletal annotations, and repair- or immune-associated processes. This study provides a segmental anatomical reference for neuro skeletal communication.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Fan Wang,Rui Xu,Xianghan Ye,Yating Zhu,Jiayin Wang,Kefei Cheng,Kaijia Xu,Yinyin Qian
Among heavy-metal-free III-V colloidal nanocrystals, Indium antimony (InSb) stands out as a promising candidate for constructing solution-processed broadband photodetectors (PDs) owing to its ultranarrow bandgap and exceptionally high carrier mobility. However, the high affinity of Sb element for oxygen makes InSb susceptible to native surface oxidation, a process that creates barriers to carrier transport and reduces light absorption efficiency, thereby significantly degrading the performance of InSb-based PDs. In this study, we propose a solution-based route for fabricating InSb nanowires (NWs) decorated with Au nanoparticles (NPs) to fabricate a broadband, self-driven PD. The incorporation of Au NPs significantly reduces the surface trap states introduced by surface native oxide layer and enhances the performance of the PD across the visible to near-infrared (NIR) region. Compared with bare InSb NWs PDs, the Au/InSb nanohybrid device achieves a dramatic improvement in the switching ratio, reaching approximately 300 under visible-to-NIR illumination at an intensity of 36 mW/cm 2 . The maximum responsivity and detectivity values of the Au/InSb nanohybrid PD were 100 times higher than those of bare InSb NWs. Finite-difference time-domain (FDTD) simulations were employed to analyze the spatial distribution of the electromagnetic field across Au/InSb nanohybrids. The localized surface plasmon resonance (LSPR) of Au NPs and the transfer of hot electrons were identified as key factors contributing to the observed performance enhancement. This study serves as a foundational exploration of the potential for high-performance PDs utilizing Au NPs and other narrow-band III-V materials exhibiting LSPR effects.
研究领域:
材料科学
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纳米技术
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光学工程
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高影响因子
危险品化学品经营许可证（带存储）