Advanced Science
·
2026
·
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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Scientific Reports
·
2026
·
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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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 31
·42780-42788
·
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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JOURNAL OF CATALYSIS
·
2026
·
IF 6
Jie Wang,Feng Gao,Jilei Lin,Chunjuan Zhang,Meiqing Shen,Linghui Kong,Gurong Shen
Ammonia is emerging as a promising carbon-free energy carrier. The electrocatalytic ammonia oxidation reaction (AOR), highly structure-sensitive, exhibits exceptional activity on Pt nanocubes (NCs) with (100) facets. Yet, synthesis methods employing metal carbonyl capping agents inevitably introduce residual metals, whose catalytic effects are often neglected. Here, Pt NCs synthesized with Mo(CO) 6 were found to contain trace Mo both in the bulk and at the surface. Surface Mo species, partially oxidized to MoO x , substantially modify the electronic structure of Pt(100), lowering activation barriers for rate-determining AOR steps and enhancing resistance to nitrogen poisoning. These effects collectively boost AOR performance, enabling a direct ammonia fuel cell with a Pt-154 anode to achieve a peak power density of 26.7 mW cm −2 . These results reveal the overlooked impact of capping-agent-derived contaminants in AOR and point to the deliberate incorporation of heterometallic modifiers as a viable strategy for advanced electrocatalyst design.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124698
·
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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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2026
·
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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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 16
·7862-7872
·
IF 3.3
Zhuhui Chen,Yue Xiong,Ranran Ma,Pei Chen,Le Duan,Shuying Yang,Ineza Urujeni Gisèle,Linjun You,Deli Xiao
To overcome the low concentration and matrix complexity of N1-methylnicotinamide (MeNam) in biological samples, this work developed a method for the detection of MeNam in urine samples using a Fe3O4@hydroxypropylmethylcellulose@2,3-dimercaptosuccinic acid (Fe3O4@HPMC@DMSA) magnetic fluid as a pre-treatment material in combination with high performance liquid chromatography. The novel adsorbent material exhibited ultra-fast adsorption kinetics and a large adsorption capacity because Fe3O4@HPMC@DMSA NPs acted as a homogeneous magnetic fluid with more varieties and quantities of interaction sites (hydrogen-bonding interaction and electrostatic interaction). The limit of determination for MeNam was 0.05 μg mL−1 with Fe3O4@HPMC@DMSA NPs. Recoveries of spiked urine samples ranged between 95.49% and 106.4%, indicating that the developed method was promising for the accurate quantification of trace amounts of MeNam in urine samples. It provides research value for the rapid assessment of the nutritional effects of NMN dietary supplements and offers a sensitive assay for metabolism studies of related functional foods.
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Small
·
2023
·Vol. 19
·期 18
·2206189
·
IF 13.3
Hanye Xing,Yonghong Song,Hao Xu,Sheng Chen,Kangkang Li,Liang Dong,Bao Wang,Jingzhe Xue,Yang Lu
Macroscopic 3D porous materials are ideal solar evaporators for water purification. However, the limited sunlight intensity and penetrating depth during solar-driven evaporation cannot prevent the biofouling formation by photothermal effect, thus leading to the deterioration of evaporation rate. Herein, a magnetic heating strategy is reported for anti-biofouling solar steam generation based on a magnetic silk fibroin (SF) scaffold with bi-heating property. Under one sun, the solar-heated top surface of magnetic SF scaffolds accelerates water evaporation at 2.03 kg m −2 h −1 , while the unheated inner channels suffer from the formation of biofilm. When exposed to alternating magnetic field (AMF), the magnetic SF scaffold can be integrally heated, leading to an efficient inner temperature to prevent biofouling in channels for water transportation. Accordingly, magneto-heated scaffolds show steady water evaporation rates after exposure to S. aureus and E. coli , which maintained 93.6–94.6% of original performance. In contrast, the evaporation rates of the scaffolds without AMF treatment are reduced to 1.31 ( S. aureus ) and 1.32 ( E. coli ) kg m −2 h −1 , decreased by 35.5% and 35.0%, respectively. In addition, the magneto-heated scaffold inhibits biofouling formation in natural lake water, maintaining 99.5% original performance.
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FUEL
·
2023
·
IF 7.4
Guang-Hui Liu,Yong-Chao Qi,Han Wang,Ai-Min Wang,Yu-Hong Kang,Yong Gao,Ni Bai,Zhan-Ku Li,Xian-Yong Wei
This paper focused on the complementary advantages of density functional theory (DFT) calculation and catalytic reaction regulation. Based on the effective identification of intermediates, the possible catalytic hydroconversion (CHC) pathways of lignite-derived aryl ethers over Ni/mordenite were discussed. Bond dissociation energy (BDE) calculations of >C–O– bonds in different substrates and intermediates show that BDEs of >C ar –O– bonds are generally higher than those of >C al –O– bonds, and there is obvious electron aggregation near O atoms. Mulliken charge distribution analyses of different atomic sites further revealed the possible adsorption sites of active hydrogen, especially H · and H + . Possible cleavage pathways were further speculated by evaluating the stability of different leaving groups. In the early stage of CHC, aromatic ring hydrogenation and >C al –O– bond cleavage dominate, rather than >C ar –O– bond cleavage. Enthalpy change analyses combined with the CHC of real substrates further indicate that lowering temperature is beneficial to the cleavage of >C ar –O– bonds under the premise of inhibiting H ··· H transfer and obtaining H · effectively. Appropriately increasing the support acidity to ensure sufficient H + release is conducive to >C al –O– bond cleavage, especially direct dehydroxylation/dehydration. The analysis of synergetic transfer pathways of active hydrogen during the CHC provides theoretical guidance for the pathway optimization of converting lignite into high-quality clean liquid fuels.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Dong Haijiao,Du Wei,Dong Jian,Che Renchao,Kong Fei,Cheng Wenlong,Ma Ming,Gu Ning,Zhang Yu
As pioneering Fe 3 O 4 nanozymes, their explicit peroxidase (POD)-like catalytic mechanism remains elusive. Although many studies have proposed surface Fe 2+ -induced Fenton-like reactions accounting for their POD-like activity, few have focused on the internal atomic changes and their contribution to the catalytic reaction. Here we report that Fe 2+ within Fe 3 O 4 can transfer electrons to the surface via the Fe 2+ -O-Fe 3+ chain, regenerating the surface Fe 2+ and enabling a sustained POD-like catalytic reaction. This process usually occurs with the outward migration of excess oxidized Fe 3+ from the lattice, which is a rate-limiting step. After prolonged catalysis, Fe 3 O 4 nanozymes suffer the phase transformation to γ-Fe 2 O 3 with depletable POD-like activity. This self-depleting characteristic of nanozymes with internal atoms involved in electron transfer and ion migration is well validated on lithium iron phosphate nanoparticles. We reveal a neglected issue concerning the necessity of considering both surface and internal atoms when designing, modulating, and applying nanozymes.
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Nano Today
·
2022
·
IF 18.962
Di Liu,Hongliang He,Fei Kong,Yixiang Cao,Fengchao Zang,Ming Ma,Ning Gu,Yu Zhang
Currently, multimodal synergistic nanoplatform emerges as an important cancer therapy paradigm, however, multimodal synergistic theranostic nanoplatform remains to be developed. Herein, using the mouse model of breast cancer, a versatile multimodal synergistic theranostic nanoplatform is rationally designed and synthesized for enhancing chemodynamic therapy (CDT), overcoming immunosuppression within tumor microenvironment , and inhibiting metastasis as well as tracking tumor. To fulfill our design, a composite Fe/Mn magnetic nanoparticle is first synthesized by loading with Fe 3 O 4 and BMS-202 (PD-L1 inhibitor) within a poly(lactide-co-glycolide)-based nanoparticle core, which are further modified with in situ synthesis of MnO 2 layer. Then, the composite metal-organic nanoparticle is coated with two targeting moieties hyaluronic acid (HA) and AMD3100 (CXCR4 antagonist), respectively, to achieve the multimodal synergistic theranostic nanoplatform ( [email protected] +AMD). With surface targeting modification, [email protected] +AMD exhibits enhanced tumor accumulation, where it effectively consumes endogenous glutathione to generate Mn 2+ allowing for the enhanced CDT effect, alleviates tumor hypoxia by O 2 generation and reverses the tumor immunosuppression. [email protected] +AMD blocks CXCR4 receptor on cancer cells, thus suppressing the CXCR4-mediated cancer metastasis and invasion. Additionally, [email protected] +AMD would synchronously be achieving tumor tracking by T 1 -T 2 dual-mode magnetic resonance imaging. Collectively, this strategy holds a novel multimodal synergistic theranostics for effective cancer management.
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Catalysts
·
2022
·Vol. 12
·期 11
·1328
·
IF 4.501
Liang-Qiu Huang,Zhi-Jun Diao,Bo Chen,Qing-Pan Du,Kai-Yang Duan,Si-Jia Zhao
Efficient depolymerization of C–O linkages is essential for converting lignin into fuels and higher value-added chemicals. In this work, CoRuP/SiO2, an amorphous Ru-Co phosphide composite, was fabricated for the efficient hydrogenolysis of ether linkages. The 4–O–5 andα–O–4 linkages containing lignin-related compounds, such as diphenyl ether, benzyl phenyl ether, 3-methyl diphenyl ether, and dibenzyl ether, are selected as representatives of linkages in lignin. Under mild conditions, Ru-containing metallic phosphides have high-performance for the catalytic depolymerization of C–O linkages. Compared with other catalysts, CoRuP/SiO2shows an outstanding selectivity for benzene and excellent efficiency in depolymerizing diphenyl ethers, yielding only a small amount of by-products. Furthermore, the total acidity shows a linear relationship with the hydrogenolysis reactivity in cleaving aromatic ether bonds. The mechanisms for the catalytic hydrogenolysis of 4–O–5 andα–O–4 bonds over CoRuP/SiO2are proposed. Moreover, two-dimensional heteronuclear single quantum coherence nuclear magnetic resonance spectroscopic analysis demonstrates that CoRuP/SiO2could effectively depolymerize C–O bonds of lignin. These dominant hydrogenolysis products from lignin have excellent potential in the production of high value-added drugs or pharmaceutical intermediates. The hydrogenolysis of lignin can be a highly efficient alternative to the existing method of lignin utilization.Keywords:hydrogenolysis;C–O linkages;metallic phosphides;reaction pathway
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