ACS Omega
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2018
·
IF 0
Yucui Hou,Zengqi Lin,Muge Niu,Shuhang Ren,Weize Wu
The conversion of abundant renewable cellulose into versatile formic acid (FA) is a potential process for efficient energy storage and application. Vanadium(V)-catalyzed oxidation with O2 in acidic aqueous media now is the most common method to realize the FA production from cellulose with both high yields and high purity. However, vanadium-based catalysts are difficult to synthesize and expensive. Thus, the seeking for cheaper catalysts with the same high efficiency is expected. In this work, after testing a variety of metal salts in acidic aqueous solution for the conversion of cellulose under O2, iron(III) was found as a cheaper and readily available catalyst for FA formation, with a comparable yield (51.2%, based on carbon) with that of vanadium(V). The effect of reaction parameters was studied. The competition between oxidation and hydrolysis was found and discussed in detail. FeCl3 and H2SO4 can accelerate oxidation and hydrolysis, respectively, whereas suppress the other. The effects can reflect on the product distribution. Intermediates were found and the pathway from cellulose to products was reasonably proposed. The reusability of the catalytic system shows good performance after four runs. The mechanism study suggests a catalytic ability by a mutual transformation between iron(III) and iron(II), where iron(III) oxidizes substrates to iron(II) that is reoxidized by O2.
研究领域:
化学
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能源科学
·
催化科学
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DOI
PubMed
Nano Research
·
2024
·
IF 9.5
Sun Yudie,Han Yunxiang,Wang Mingyue,Ye Mingfu,Wu Konglin,Zhang Kui
Circulating microRNAs (miRNAs) play a pivotal role in the occurrence and development of acute myocardial infarction (AMI), and precise detection of them holds significant clinical implications. The development of luminol-based luminophores in the field of electrochemiluminescence (ECL) for miRNA detection has been significant, while their effectiveness is hindered by the instability of co-reactant hydrogen peroxide (H 2 O 2 ). In this work, an iron single-atom catalyst (Fe-PNC) was employed for catalyzing the luminol-O 2 ECL system to achieve ultra-sensitive detection of myocardial miRNA. Target miRNA triggers a hybridization chain reaction (HCR), resulting in the generation of a DNA product featuring multiple sticky ends that facilitate the attachment of Fe-PNC probes to the electrode surface. The Fe-PNC catalyst exhibits high promise and efficiency for the oxygen reduction reaction (ORR) in electrochemical energy conversion systems. The resulting ECL biosensor allowed ultrasensitive detection of myocardial miRNA with a low detection limit of 0.42 fM and a wide linear range from 1 fM to 1.0 nM. Additionally, it demonstrates exceptional performance when evaluated using serum samples collected from patients with AMI. This work expands the application of single-atom catalysis in ECL sensing and introduces novel perspectives for utilizing ECL in disease diagnosis.
研究领域:
生物传感器
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电化学
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纳米技术
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心脏病学
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分子诊断
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DOI
高影响因子
PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2024
·Vol. 44
·期 5
·1951-1969
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IF 2.6
Siyuan Sui,Guohua Ni,Hongmei Sun,Ling Kong,Tao Sun
In this paper, a novel method is presented to enhance the antimicrobial properties of polyvinyl chloride (PVC) via plasma-induced grafting of quaternary ammonium (QA). The results show that the content of oxygen-containing functional groups on PVC surface is significantly increased after Ar-O 2 plasma treatment, beneficially enhancing the thickness and adhesion of QA coating. Plasma treatment time critically affects the morphology of PVC surface, which is closely related to the number, depth and diameter of pit on the surface. With the increase of pits size, the PVC surface forms ridge-like protrusions. The coating formed by grafting QA maintains the morphology characteristics of plasma-treated PVC surface. Results of antibacterial test show that specimens have the best antibacterial activity when there are a high and sharp ridge-like structure of QA coating on the plasma-treated PVC surface.
研究领域:
生物材料学
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表面科学
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高分子化学
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抗菌材料
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医学工程
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
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IF 3.779
Yunzhao Liu,Xiaowei Chi,Qi Han,Yuexiu Du,Jianhua Yang,Yu Liu
Sodium–oxygen (Na−O 2 ) batteries are being extensively studied because of their higher energy efficiency and lower cost compared to those of lithium–oxygen (Li–O 2 ) batteries. However, highly efficient and durable cathode catalysts are very limited, thus considerably hindering the application of Na–O 2 batteries. Herein, a vertically self-standing C@NiCo 2 O 4 nanoneedle arrays (C@NiCo 2 O 4 -NAs) have been delicately designed and fabricated by a facile hydrothermal method . The NiCo 2 O 4 nanoneedles are in-situ grown on the carbon paper , forming an unique urchin-like structure, which is directly used to Na–O 2 batteries as a self-standing and binder-free cathode for the first time. Under a current density of 50 mA g −1 , the Na–O 2 battery containing C@NiCo 2 O 4 -NAs cathode shows a high initial discharge capacity of 6500 mAh g −1 (based on NiCo 2 O 4 material mass) and low over-potential of 0.6 V due to the numerous catalytic sites and high electron mobility of C@NiCo 2 O 4 -NAs. SEM, XPS and FTIR tests have confirmed the formation of thin film-like Na 2 O 2 discharge product on the surface and gaps of NiCo 2 O 4 nanoneedles, and the special film-like structure can facilitate the decomposition of Na 2 O 2 in the subsequent charging process and reduce the over-potential notably. Meanwhile, the robust urchin-like structure of C@NiCo 2 O 4 -NAs renders the Na–O 2 battery a high cyclic stability up to 120 cycles when the specific capacity is limited to be 800 mAh g −1 .
研究领域:
储能
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材料科学
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电化学
·
纳米材料
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yaying Dou,Xin-Gai Wang,Dashuai Wang,Qinming Zhang,Chengyi Wang,Gang Chen,Yingjin Wei,Zhen Zhou
Large overpotential in oxygen reduction and evolution reactions is the intractable obstruction of Li-O 2 batteries, causing inferior round-trip efficiency and diminished cycle life. Modulating the reaction mechanism of Li 2 O 2 is of crucial importance for a high-performance Li-O 2 battery. Herein, we report a composite of amorphous RuO 2 nanoparticles decorated carbon nanotubes (A-RuO 2 @CNT) as an efficient catalyst for Li-O 2 batteries. The amorphous catalyst contains abundant defects and vacancies as well as distorted atom arrangements, which provide sufficient active sites for reactions and enhance the affinity for LiO 2 intermediates. As a result, the formation/decomposition mechanisms of Li 2 O 2 are reasonably regulated. An amorphous film-like Li 2 O 2 product forms and uniformly deposits on the surface of A-RuO 2 @CNT, thus achieving faster redox kinetics and smaller overpotential. When used in Li-O 2 batteries, the amorphous catalyst affords remarkably decreased charge overpotential and enhanced cyclic stability, which is superior to its crystalline counterpart.
研究领域:
储能
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电化学
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材料科学
·
纳米材料
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Linna Dai,Xin Zhou,Yuan Yang,Pei Hu,Lijie Ci
Nonaqueous Li − O 2 battery (LOB) is considered one of the most promising energy storage system due to its ultrahigh theoretical specific capacity (3500 Wh kg −1 ). Introducing vacancies in CoMn 2 O 4 catalysts is regarded as an effective strategy to enhance the electrochemical performances of LOB. However, the relation between vacancy types in CoMn 2 O 4 and catalytic performances in the LOB remains ambiguous. Herein, ordered porous CoMn 2 O 4 with oxygen and metal vacancies is obtained via solvothermal reaction followed by temperature-controlled calcination using polystyrene spheres as templates. The increase in treatment temperature reduces the content of oxygen vacancies while increasing that of the metal vacancies. Notably, experimental results and theoretical calculations show that oxygen vacancies in CoMn 2 O 4 have a greater influence than metal vacancies in modulating the LiO 2 adsorption during the reaction processes and reducing the overpotential. CoMn 2 O 4 synthesized at 500 ℃ (CoMnO-500) with higher oxygen vacancies exhibits stronger adsorption onto the LiO 2 , facilitating the formation of film-like Li 2 O 2 . Therefore, an LOB with the CoMnO-500 catalyst presents the lowest overpotential of 1.2 V and longest cycle lifespan of 286 cycles at a current density of 200 mA g −1 . This study offers insights into the effect of CoMn 2 O 4 vacancies on the formation pathway of Li 2 O 2 discharge products.
研究领域:
材料科学
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电化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Linlin Xie,Xingye Ma,Zheng Wang,Caifang Wang,Zhongxin Xiao,Ling-Dong Sun,Chun-Hua Yan,Chen-Jie Fang
Pyroptosis resulted from photodynamic therapy (PDT) plays a crucial role in triggering photoimmunotherapy (PIT). However, visible light-triggered PDT may rise phototoxicity, with low penetration into biological tissues. Crucially, the efficacy of PDT in eliciting pyroptosis remains suboptimal. To address these formidable challenges, we developed a O 2 -supplementing photosensitizer AuNCs@TAT that could efficiently induce pyroptosis upon irradiation with second near-infrared (NIR-II) light in hypoxic tumor microenvironment (TME). Replacing GSH with TAT resulted in a gold nanocluster AuNCs@TAT. The ratio of Au (I) to Au (0) shifted from 1: 0.26 in pristine AuNCs to 1: 1.21 in AuNCs@TAT, which contributed to enhanced catalytic activity of AuNCs@TAT. The superior catalase-like activity of AuNCs@TAT produced 1.9-fold higher O 2 than AuNCs. This O 2 self-supplying capability of AuNCs@TAT not only relieved hypoxic condition in TME but also significantly enhanced the efficiency of AuNCs@TAT to induce pyroptosis upon 1064 nm light irradiation. Western blotting indicated both remarkable upregulation of cleft Caspase-3 and GSDME-N, suggesting GSDME mediated pyroptosis. Further, release of pro-inflammatory cytokines and damage-associated molecular patterns (DAMPs) triggered a strong systematic immune response and reprogrammed the immunosuppressive microenvironment into an immunostimulatory state, which led to a significant suppress of tumor metastasis in mice. Overall, this work sets the stage for future advancements in the design of NIR-II photosensitizer with O 2 -supplementing capability and therefore offers an innovative framework and solid foundation for tumor PIT.
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产品关联
DOI
高影响因子
Theranostics
·
2026
·Vol. 16
·期 6
·2811
·
IF 13.3
Hanqing Zhao,Wenjun Shao,Man Jiang,Fangyuan Chen,Yingying Li,Xiaoyu Zhang,Tao Ma,Minglong Chen,Baohong Sun,Zekun Wang,Chuanbin Wu,Qingqing Wang
Rationale: Chronic diabetic wounds present significant therapeutic challenges due to biofilm resistance and dysregulated metabolism of glucose, reactive oxygen species (ROS), and nitric oxide (NO), which collectively exacerbate immunosuppression and impair tissue repair. Methods: This study developed a glucose-driven cascade nanozyme-loaded dissolvable microneedle system (PPLG@MN) that enables spatiotemporal regulation of the wound microenvironment through a closed-loop mechanism involving nutrient deprivation, gas modulation, and immune reprogramming. The system consists of porous Prussian blue nanozymes (PPB) loaded with glucose oxidase (GOx) and L-arginine (L-arg), which is precisely delivered into the tissue via microneedles. Results: PPLG@MN initiates a self-sustaining therapeutic cycle within the biofilm microenvironment, in which GOx catalyzes the oxidation of glucose to generate hydrogen peroxide (H 2 O 2 ), inducing bacterial starvation. Subsequently, H 2 O 2 reacts with PPB and L-arg to release oxygen (O 2 ) and biofilm-disrupting NO, thereby alleviating local hypoxia and enhancing antibacterial efficacy. Furthermore, the synergistic action of O 2 and NO reprograms macrophages toward an anti-inflammatory M2 phenotype (approximately 30-fold increase compared to the model group), effectively resolving inflammation and promoting angiogenesis. In vivo studies confirmed that the system achieved > 99.9% biofilm eradication efficiency and accelerated wound healing by 25.6% compared to the model group. Conclusion: This nanoplatform offers a clinically translatable therapeutic strategy for biofilm-associated diabetic wounds by synergistically combining gas therapy and immune reprogramming.
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产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2026
·
IF 6.6
Chunke Zhao,Yueying Gao,Jiaye Duan,Shiting Li,Bo Zhang,Ke Ma,Longtao Dang,Gen Wang
Polymeric removal of various FPs with concurrent defluorination is achieved in a CuO/PMS system. • FPs are efficiently converted into solid PPO-like polymers with minimal PMS consumption. • 1 O 2 and O 2 •− synergistically drive the polymerization and defluorination of FPs. • Continuous-flow operation over 120 h sustains ∼95% 4-FP removal, confirming practical applicability. Fluorophenols (FPs) are persistent organic pollutants of high concern owing to the extreme stability of their C F bonds. Here we report an oxidative polymerization strategy that enables simultaneous pollutant removal and defluorination by transforming FPs into solid polymers. In a CuO-activated peroxymonosulfate (PMS) system, a superoxide radical (O 2 •− ) and singlet oxygen ( 1 O 2 ) co-mediated oxidation process was established. The system achieved near-complete removal of a series of FPs with different fluorine substitution patterns (2-FP, 4-FP, 2,4-DFP, and 2,3,5,6-TeFP) using minimal oxidant consumption. Polymerization efficiencies ranged from ∼26% to ∼72%, accompanied by significant defluorination (up to ∼74%). Mechanistic studies reveal that FPs are converted into solid poly(phenylene oxide)-like polymers via a nucleophilic aromatic substitution route. Beyond batch performance, the system demonstrated excellent practical viability, with ∼95% removal of 4-FP sustained in a continuous-flow reactor and defluorination remaining as high as ∼47% after prolonged operation. The process also maintained high efficiency under hypersaline and complex water matrices. This integrated defluorination-polymerization approach offers a cost-effective, environmentally benign and operationally stable solution for treating FPs-contaminated wastewaters, shifting the paradigm from conventional mineralization toward sustainable resource recovery. Download: Download high-res image (163KB) Download: Download full-size image
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Jing Lan,Yuran Yu,Luyao Xing,Fujun Miao,Guosheng Shao,Peng Zhang
Self-supporting Cu/TiN nano-furry serves as a superior bifunctional catalyst for ORR/OER. • DFT reveals Cu/TiN heterojunctions facilitate uniform Li 2 O 2 film growth via enhanced LiO 2 affinity. • Carbon-free catalytic system effectively suppresses Li 2 CO 3 byproduct formation, reducing overpotential. • Delivers ultralow overpotential, high areal capacity and superior stability, outperforming Au-based counterparts. The major hindrance against developing high-performance lithium oxygen batteries (LOBs) lies in their infamously sluggish redox kinetic processes involving undesirable parasitic reactions, which results in large overpotential, low capacity and inferior cycling stability. The rational catalyst design is proposed as an efficient strategy to address the above issue. Herein, we have developed a self-supporting nano-furry cathode based on a Cu foam-supported hierarchical nanotube array architecture decorated with Cu/TiN nanojunctions, which contributes to a fresh bifunctional catalytic mechanism for enhancing ORR/OER catalytic kinetics. Such an integrated cathode with Cu/TiN nanojunctions catalyst enables resilient LOBs through minimizing the energy barriers and excessive input energy to form/decompose Li 2 O 2 , outperforming similar Au-based system. DFT simulation elaborates that the Cu-based heterojunctions with favorable LiO 2 -affinity tend to promote surface deposition of uniform Li 2 O 2 film, alleviating disproportionated reaction and achieving remarkably enhanced capacity. Consequently, this rationally designed cathode for LOBs achieved high area capacity up to 25.6 mAh cm −2 with a small overpotential of 0.37 V at 0.1 mA cm −2 , and exceptional cycle stability with over 350 cycles at 0.2 mA cm −2 under a fixed capacity of 0.25 mAh cm −2 . This work provides an insightful approach towards designing efficient, clean and cheap cathode with abundant metal-based catalysts for LOBs. Download: Download high-res image (278KB) Download: Download full-size image
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DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Sipeng Tian,Baobing Tang,Mingzi Sun,Zhangpeng Xu,Tongtong Zhai,Huanhuan Xing,Bolong Huang,Yunling Liu,Jing Li,Erkang Wang
Classic luminol-H2O2 chemiluminescence (CL) systems are plagued by inherent self-decomposition, which compromises detection reliability. Although luminol-dissolved oxygen systems circumvent this issue, their ultralow reactivity necessitates innovative catalytic microreactor design. Herein, we pioneer a hydrogen-bonded organic framework (HOF) constructed from metal–organic square units and 1,2-propanediamine ligands as terminal hydrogen-bonding sites, achieving an unprecedented 4284-fold CL enhancement in luminol-O2 systems. HOF with porous zeolite-like supramolecular assemblies (ZSA) serves as the coreaction accelerator with strong O2 adsorption at tetrahedral Co–N/O sites that activates O2 to generate reactive oxygen species (ROS). And the kinetic confinement effect provided by the ZSA host with suitable channel and hydrogen-bonding contributions efficiently captured the luminol emitter in the nanocages, shortening electron-transfer pathways and reducing nonradiative energy loss. And the synergistic confinement catalysis enhanced CL performance is linearly related to the O2 adsorption capacity of the ZSA series (ZSA-1, ZSA-3, and ZSA-4). Theoretical calculations further confirmed that the adsorption of O2 and luminol in ZSA-1 optimizes the electron-transfer pathways to promote CL emission performances compared with those of zeolitic imidazolate framework-67 (ZIF-67). This work not only expands the application of HOF in the field of CL but also provides new insights for engineering materials to boost the CL photon emission efficiency of weak luminol-O2 systems.
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Shanjian Liu,Jia Liu,Wenjing Zhao,Wei Chen,Chengxizi Zhang,Weiming Yi
To synergistically achieve industrial flue gas resourcing and high-value biomass conversion, a novel process of cellulose-catalyzed nitrogen-rich pyrolysis mediated by oxygen-poor flue gas was proposed in this paper. A systematic investigation of the influences of O 2 concentration (1–7 vol%), temperature (450–600 °C), and the presence of Al-MCM-41 on the cellulose-urea co-pyrolysis for preparing nitrogen-containing compounds (NCCs) was conducted. Under optimal conditions (550 °C, 5 vol% O 2 ), the synergistic effect of mesoporous structure and acid sites of Al-MCM-41 transformed the product distribution from levoglucosan-dominated oxygenated compounds to high-value NCCs mainly comprising nitriles (25.3 %) and pyrazines (25.2 %). The relative content of NCCs reached 92.1 %, showing a 46.1 % increase compared to non-catalytic conditions. The process opens up a green and efficient synergistic path for the co-conversion of industrial waste gas and biomass, demonstrating significant industrial application value.
研究领域:
能源与环境科学
·
催化化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）