ACS Omega
·
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
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催化科学
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DOI
PubMed
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Bingbing He,Qinyuan Wang,Ying Chen,Weifeng Yao
The development of a cost-effective method for synthesizing hydrogen peroxide (H2O2) holds significant importance. Here, we introduce a novel catalyst, a nitrogen-doped carbon-loaded nickel nanoparticle catalyst (Nix NPs@N–C), tailored for efficient H2O2 production via the two-electron oxygen reduction reaction. Benefiting from the synergistic interplay between highly active nickel nanoparticles and nitrogen-doped carbon, the optimal Nix NPs@N–C catalyst demonstrates an outstanding 78% selectivity for H2O2 at 0.5 V vs a reversible hydrogen electrode (RHE), yielding approximately 387 mmol g–1 h–1 in a 0.1 M KOH alkaline solution at 0.3 V vs RHE. With its utilization of cost-effective raw materials, streamlined synthesis method, and exceptional catalytic performance, the Nix NPs@N–C catalyst emerges as a promising candidate for electrocatalytic H2O2 synthesis in practical applications.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS ENGINEERING AND PERFORMANCE
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2025
·
IF 2
Zhang Dongbo,Tang Xinyue,Wang Ning,Xiao Mingwei,Yan Jiangrong,Zhang Yongsheng
High-entropy oxides used as thermal barrier coating materials have attracted considerable attention from scientific communities owing to their unique properties, such as low thermal conductivity and good stability at high temperatures. In this study, a new (La 0.2 Gd 0.2 Zr 0.2 Ce 0.2 Ho 0.2 )O 2-δ ((LGZCH)O) fluorite-structured high-entropy oxide was successfully synthesized through a solid-state reaction at 1400 °C. The resulting material demonstrated good phase stability after sintering at high temperatures. The microstructure, microscopic morphology, ionic valence, compositional distribution, optical properties, thermal conductivity, thermal expansion properties, and mechanical properties of (LGZCH)O were investigated. X-ray diffraction results showed that the (LGZCH)O fluorite-structured high-entropy oxide exhibited good stability during sintering at different temperatures with an optimum sintering temperature of 1580 °C. Ce 4+ converted to Ce 3+ at high temperatures. Scanning electron microscopy results showed that the material had a high porosity of approximately 28.9% after sintering at 1580 °C. (LGZCH)O had a higher infrared radiation emissivity of 82.2%-87.6% in the range of 2.5-6.0 μm indicating that it had better thermal radiation shielding performance. After porosity modification, the thermal conductivity ranged from 1.27 to 1.00 W m −1 K −1 from room temperature to 1000 °C, which is considerably lower than that of yttria-stabilized zirconia. Additionally, (LGZCH)O exhibited low coefficients of thermal expansion measuring 9.65 × 10 −6 K −1 and 10.13 × 10 −6 K −1 at 1000 and 1200 °C, respectively. The hardness and Young’s modulus of the bulk (LGZCH)O measured via nanoindentation tests were 8.86 GPa and 153.98 GPa, respectively, which are marginally inferior to those of YSZ. Therefore, (LGZCH)O can be considered a promising candidate material for thermal barrier coatings.
研究领域:
材料科学
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能源工程
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
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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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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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
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催化化学
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产品关联
DOI
高影响因子
Communications Chemistry
·
2025
·Vol. 8
·期 1
·389
·
IF 6.2
Han Lei,Tan Jingying,Zhang Yucui
Given the promising prospect of nanozymes in colorimetric test strips, it is essential to eliminate the interferences of their multi-activities and various colors on the test strip. Here, white Mn-based metal-organic frameworks (Mn-MOFs) with ultrathin 2D morphology (3 nm thick) were successfully synthesized by a simple ultrasonic approach. The origin of the white optical property in Mn-MOFs was systematically investigated, revealing that it stems from specific metal-ligand coordination polymerization rather than morphological features or defect states. Mn-MOF nanozymes possessed exclusive peroxidase-mimicking activity rather than oxidase-like activity, effectively resisting O 2 interference during colorimetric assay. Moreover, Mn-MOF nanozymes displayed unique substrate selectivity without additional modification. Unlike other colored nanozymes, the whiteness of Mn-MOF nanozymes enhanced the paper’s whiteness, boosting contrast for colorimetric detection on test strip. This study pioneers a systematic investigation into the origin of whiteness in MOF nanozymes. The coordination-defined properties enable interference-free optical design and O 2 -resistant on-site detection.
研究领域:
材料科学
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纳米技术
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分析化学
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生物传感器
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酶模拟
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·Vol. 60
·期 48
·25148-25163
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IF 3.9
Zhang Zhenyan,Chai Huan,Yu Zhengqian,Li Jinsheng,Li Pengfei,Wu Lei,Li Zhanshuai,Qi Xiwei
TiO 2 -based materials are widely used in high-temperature capacitors and aerospace electronics but face challenges such as high dielectric loss and limited thermal stability in conventional single-component systems. To address these issues, we propose a novel strategy integrating high-entropy doping design and oxygen vacancy engineering. In 2 O 3 -doped (GeMnTiSnMo)O 2 high-entropy ceramics (GMTSMO- x In, x = 0.1–1) were synthesized via solid-state reaction. Experimental results reveal that In 3+ doping generates high-density oxygen vacancies (V o ·· ) through charge compensation, forming [Ti 3+ - V o ·· -Ti 3+ ] and [Mn 3+ - V o ·· -Mn 3+ ] defect-dipole clusters. These clusters enhance electron localization and suppress carrier migration, reducing dielectric loss by threefold. Simultaneously, oxygen vacancy enrichment strengthens interfacial polarization, increasing the dielectric constant by fourfold. The optimal GMTSMO-0.5In exhibits a relative permittivity ( ε r ) of 4.0 × 10 6 and a low loss tangent of 15 at 650 ℃/100 Hz, outperforming traditional TiO 2 -based materials and existing high-entropy oxides. All compositions demonstrate excellent temperature stability (25–400 ℃) and frequency-independent behavior above 10 4 Hz. This work provides a high-entropy-driven approach for dynamic defect engineering, paving the way for advanced dielectric materials in extreme-condition energy storage systems.
研究领域:
材料科学
·
陶瓷与介电材料
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电子材料
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储能技术
·
缺陷化学
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产品关联
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
BIOSENSORS & BIOELECTRONICS
·
2019
·
IF 9.518
Zepeng Kang,Yi-Heng P. Job Zhang,Zhiguang Zhu
In this study, a novel carbon tube was prepared by carbonizing a rectangular polypyrrole (RPPy) tube at a high temperature for the construction of enzymatic biofuel cells with high performance. SEM and TEM images clearly showed that the initial PPy presented a rectangular tube shape, while the carbonized PPy became a shriveled rectangular tube with a concave surface, which might be beneficial for enzyme immobilization and electrochemical applications. The glucose oxidase (GOx)- or laccase (Lac)-modified electrodes based on carbonized RPPy exhibited excellent bioelectrochemical performance. In addition, a biofuel cell (GOx, glucose/O 2 , Lac) was assembled, and the open-circuit voltage reached 1.16 V. The maximum power density was measured to 0.350 mW cm −2 , which correlated to the gravimetric power density of 0.265 mW mg −1 (per mg of GOx) at 0.85 V. The constant-current discharge method was used to further evaluate the continuous discharge capacity. The discharge time reached 49.9 h at a discharge current of 0.2 mA before the voltage was lower than 0.8 V. Furthermore, three of the fabricated biofuel cells in series were able to continually light up a white light-emitting diode (LED) whose turn-on voltage was ca. 2.4 V for more than 48 h. This study suggests that carbonized conducting polymers may become a useful electrode material for the development of enzymatic biofuel cells.
研究领域:
生物化学
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材料科学
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能源科学
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DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Yiqiao Wang,Siyuan Pan,Yong Guo,Shichao Wu,Quan-Hong Yang
Li-O 2 batteries require catalysts to solve the problem of sluggish oxygen-related reaction kinetics. However, the solid catalysts and redox mediators are intrinsically deficient due to poor solid contacts and shuttle problems, respectively. Here, we report lithium phthalimide-N-oxyl (LiPINO) as a phase transfer catalyst (PTC) for promoting Li 2 O 2 formation and its reversible decomposition through the solution-phase reactions. The interaction between LiPINO and oxygen species in the electrolyte enables the high dissolution and stability of oxygen species, the fast charge transfer at liquid-solid interfaces and superior kinetics, and the suppressed side reactions. The efficient bidirectional catalytic activity and high stability of LiPINO capacitate batteries with a highly improved discharge capacity (11400 mAh g −1 ), a largely lowered charge potential (3.14 V) and an extended cycle life (more than 200 cycles) both in O 2 and air. Our understanding of the phase-transfer catalysis towards the Li-O 2 electrochemistry and the discovery of the PTC with superior activity and stability provide deep insights into the design of the most reliable catalysts for Li-O 2 batteries.
研究领域:
电化学
·
能源材料
·
物理化学
·
电池技术
·
催化化学
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DOI
高影响因子
ADVANCED MATERIALS
·
2024
·
IF 27.4
Shuyu Wang,Miaomiao Cheng,Shenghui Wang,Wei Jiang,Feifei Yang,Xiaomei Shen,Lirong Zhang,Xiyun Yan,Bing Jiang,Kelong Fan
Radiotherapy (RT), essential for treating various cancers, faces challenges from tumor hypoxia, which induces radioresistance. A tumor-targeted “prosthetic-Arginine” coassembled nanozyme system, engineered to catalytically generate nitric oxide (NO) and oxygen (O 2 ) in the tumor microenvironment (TME), overcoming hypoxia and enhancing radiosensitivity is presented. This system integrates the prosthetic heme of nitric oxide synthase (NOS) and catalase (CAT) with NO-donating Fmoc-protected Arginine and Ru 3+ ions, creating HRRu nanozymes that merge NOS and CAT functionalities. Surface modification with human heavy chain ferritin (HFn) improves the targeting ability of nanozymes (HRRu-HFn) to tumor tissues. In the TME, strategic arginine incorporation within the nanozyme allows autonomous O 2 and NO release, triggered by endogenous hydrogen peroxide, elevating NO and O 2 levels to normalize vasculature and improve blood perfusion, thus mitigating hypoxia. Employing the intrinsic O 2 -transporting ability of heme, HRRu-HFn nanozymes also deliver O 2 directly to the tumor site. Utilizing esophageal squamous cell carcinoma as a tumor model, the studies reveal that the synergistic functions of NO and O 2 production, alongside targeted delivery, enable the HRRu-HFn nanozymes to combat tumor hypoxia and potentiate radiotherapy. This HRRu-HFn nanozyme based approach holds the potential to reduce the radiation dose required and minimize side effects associated with conventional radiotherapy.
研究领域:
肿瘤学
·
纳米技术
·
生物化学
·
治疗学
·
放射肿瘤学
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DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2022
·Vol. 34
·期 40
·2201838
·
IF 32.086
Guiru Sun,Rui Gao,Hailiang Jiao,Dan Luo,Yan Wang,Zexu Zhang,Wei Lu,Ming Feng,Zhongwei Chen
The major challenges for Li-O 2 batteries are sluggish reaction kinetics and large overpotentials due to the cathode passivation resulting from insulative and insoluble Li 2 O 2 . Here, a novel nanodot (ND)-modified electrolyte is designed by employing cobalt bis(trifluoromethylsulfonyl)imide (Co(TFSI) 2 ) as an electrolyte additive. The Co(TFSI) 2 additive can react with discharge intermediate LiO 2 and product Li 2 O 2 to form CoO NDs. The generated CoO NDs are well dispersed in electrolyte, which integrates both the high catalytic activity of solid catalyst and the good wettability of soluble catalyst. Under the catalytis of CoO NDs, Li 2 O 2 is produced and deposits on the cathode together with them. At the recharge process, these well dispersed CoO NDs help to decompose solid Li 2 O 2 at a lower overpotential. The Li-O 2 cells with Co(TFSI) 2 exhibit a long cycle life of 200 cycles at a current density of 200 mA g −1 under a cutoff capacity of 1000 mAh g −1 , as well as a superior reversibility associated with the Li 2 O 2 formation and decomposition. The study is expected to broaden the range of electrolyte additives and provide a new view to developing highly dispersed NDs-based catalysts for Li-O 2 batteries.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）