CARBON
·
2019
·
IF 7.466
Dan Cheng,Zhe Wang,Chang Chen,Kebin Zhou
Constructing efficient bifunctional oxygen electrocatalyst which integrates highly efficient active sites with desired structures for rapid mass transport is of great importance for designing rechargeable Zn-air battery with high power density and fast charge and discharge performances. Herein, defect-enriched N-doped graphitic carbon microspheres with fully open and 3D interconnected super-macropores are successfully constructed by an elaborate coating-activation synthesis strategy. The resulted novel structures are featured with abundant defects as active sites and bicontinuous structures, i.e. , the continuous carbon skeleton and the interconnected super-macropores for fast electron and mass transport, respectively. Our synthesized defect-enriched N-doped graphitic carbon microsphere bifunctional oxygen electrocatalysts display excellent performance. The rechargeable Zn-air batteries exhibit a long time charging-discharging cycles as long as 800 cycles at even 50 mA cm −2 . This study provides an attractive guide to improve the bifunctional oxygen catalytic performances and promote the Zn-air battery applications in both electric vehicles and grid energy storage in the future.
研究领域:
材料科学
·
能源存储与转换
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Haichao Yu,Xuan Chen,Jie Zhou,Hui Wang,Shanshan Qiu
At present, responsible disposal of scrapped lithium-ion batteries (LIBs) is crucial to address the global issues of electronic waste. Herein, we propose an eco-friendly one-step technology to convert spent graphite (SG) in LIBs to nitrogen-doped defect-enriched graphite (NG) with an NH 4 Cl roasting strategy. This recycling technique does not require leaching by acids or water, and accordingly is free of any complicated separation processes. Detailed material analysis and experimental study demonstrated that our strategy not only removes most of the impurities in spent graphite, but also introduces extrinsic defects into the graphite matrix, leading to enhanced reversible Li + storage and cycling stability. The NG delivers a remarkably improved reversible specific charge capacity of 455.9 mAh g −1 for the 1st cycle, and 452.1 mAh g −1 after 50 cycles at 0.1 A g −1 with nearly no attenuation, and also exhibits a desirable rate performance (a capacity of 175.3 mAh g −1 is achieved at 2 A g −1 ), in comparison to the SG and the commercial natural flake graphite (CG). This study offers a new viewpoint on the recycling technology of graphite anodes using in situ nitrogen doping for graphite, and meaningful progress toward the sustainable development of LIBs.
研究领域:
材料科学
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环境科学
·
能源技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xuan Luo,Lingrui Zhang,Xiaobo Gong,Yong Liu,Jing Tian
The removal of antibiotics from wastewater is crucial, and the activating of PMS is an effective method for this purpose. To design a suitable catalyst, a defect-enriched ilmenite-type catalyst (D-FeTiO 3 /C) was constructed using titanium dioxide slag as a precursor for peroxymonosulfate (PMS) activation to remove tetracycline (TC). The obtained D-FeTiO 3 /C catalyst showed excellent activation ability towards PMS, achieving a TC degradation efficiency over 90% within 120 min. The introduction of oxygen vacancies by ball milling significantly improved the activation ability. The effects of operational conditions on TC removal were systematically investigated in the D-FeTiO 3 /C/PMS system. The primary active species in the D-FeTiO 3 /C/PMS system were non-free radicals of singlet oxygen, although free radical species also contributed to TC degradation. Degradation pathways for TC were proposed, and most of the intermediates were non-toxic by-products. This study developed a promising method to recycle solid slag wastes and effectively treat antibiotics in water environments.
研究领域:
环境科学
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催化化学
·
废水处理
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Ming Wu,Libo Chen,Ying Sheng,Lizhi Song,Hu Zhou,Jian Jian,Tiefan Huang,Botian Liu,Xiaoning Li
The limited efficiency of traditional photocatalysts necessitates innovative solutions for sustainable hydrogen production. In this study, a three-dimensional (3D) sponge-like porous carbon nitride (SCN-x) was successfully synthesized using a novel method involving the removal of unstable organic frameworks. The resulting SCN-x exhibits a highly interconnected network structure and significantly higher surface area (116.5 m 2 /g), compared to normal pure carbon nitride (PCN). Furthermore, this method introduces significant defects into SCN-x, such as additional foreign oxygen atoms, which not only modulate its band structure but also provide more active sites at the defects. These features increase the number of photo-induced electron-hole pairs due to enhanced light absorption, and suppresses their recombination by enabling them to efficiently participate in the reaction with increased number of active sites. As a result, compared to PCN, the optimal SCN-0.5 sample exhibits 86.6 times higher photocatalytic hydrogen production rate under visible light irradiation, along with excellent stability and a high apparent quantum yield (AQY) of 5.8 % under 420 nm illumination. Furthermore, with additional calcination under air, the 2SCN-0.5 sample delivers a record-high hydrogen evolution rate of 1663.5 μmol∙h −1 ∙g −1 under natural sunlight irradiation. This work presents a novel method for preparing a metal-free photocatalyst by introducing significant defects and a high surface area, enabling efficient large-scale hydrogen production under natural sunlight.
研究领域:
材料科学
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能源科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2022
·
IF 12.92
Shi-Qun Cheng,Xue-Fei Weng,Qing-Nan Wang,Bai-Chuan Zhou,Wen-Cui Li,Ming-Run Li,Lei He,Dong-Qi Wang,An-Hui Lu
Copper-based heterogeneous catalysts commonly exhibit uncontrolled growth of copper species under reaction conditions because of the low Hüttig temperature (surface mobility of atoms) and Tamman temperature (bulk mobility) for copper at just 134 and 405 °C, respectively. Herein, we report the use of defect-enriched hexagonal boron nitride nanosheets (BNSs) as a support to anchor the Cu species, which resulted in superior dispersion of the Cu species. The obtained Cu/BNS catalyst was highly stable for ethanol dehydrogenation , with a high selectivity of 98% for producing acetaldehyde and an exceptionally high acetaldehyde productivity of 7.33 g AcH g cat –1 h –1 under a weight hourly space velocity of 9.6 g EtOH g cat –1 h –1 . The overall performance of our designed catalyst far exceeded that of most reported heterogeneous catalysts in terms of the stability of the Cu species and the yield of acetaldehyde in this reaction. The hydroxyl groups at the defect edges of BNS were responsible for the stabilization of the copper species, and the metal-support interaction was reinforced through charge transfer, as evidenced by coupling atomic resolution images with probe molecule infrared spectroscopy and X-ray photoelectron spectroscopy. A designed in situ diffuse reflectance infrared Fourier transform spectroscopy study of ethanol/acetaldehyde adsorption further revealed that Cu/BNS favored ethanol adsorption while suppressing acetaldehyde adsorption and further side reactions. This study demonstrates a new method for designing highly dispersed Cu-based catalysts with high durability.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Advanced Optical Materials
·
2021
·Vol. 10
·期 1
·2101669
·
IF 9.926
Zhihao Zhou,Shuai Zhang,Yakun Le,Hong Ming,Yang Li,Shi Ye,Mingying Peng,Jianrong Qiu,Guoping Dong
Spinel configuration is a kind of broadly considered host candidate when designing persistent luminescence (PersL) materials due to the easy generation of vacancies and anti-site defects. Here, a new strategy of defect enrichment for the activation of PersL is proposed, and in contrast to the spinel configuration, it is demonstrated that the crystal structure of near inverse spinel ensures more numerous defects to activate the near-infrared (NIR) PersL of Fe 3+ . Fe 3+ -doped MgGa 2 O 4 displays the PersL band in the range of 600 to 900 nm and possesses a super-long PersL duration time >15 h. The optical analysis and the calculation of density functional theory unravel that the near inverse spinel structure can lower the carrier transfer barriers to accelerate the formation of carrier trap states within the bandgap. Therefore, more numerous defects in this structure may participate in the trapping and de-trapping process by comparison with the normal spinel configuration. These findings are expected to accelerate the development of new PersL materials through Fe 3+ doping toward versatile biological applications in NIR window.
研究领域:
材料科学
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光学物理
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生物医学工程
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DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 12
·6748-6761
·
IF 14.511
Guangyao Li,Yanqi Xu,Hong Pan,Xiangli Xie,Rongrong Chen,Di Wu,Linjiang Wang
Vanadium-based catalysts have long been applied in arene Csp2–H bond activation and functionalization, but enormous challenges remain in terms of high activity, selectivity, and stability. Herein, defect-enriched NiV-layered double hydroxide nanosheets (NiV-LDH-NS) with a bimetallic synergistic effect were prepared by a one-step co-precipitation strategy as an electrocatalyst for phenol hydroxylation. The appropriate valence band of NiV-LDH-NS could provide a suitable thermodynamic driving force in electrochemical phenol hydroxylation and simultaneously avoid overoxidation. X-ray absorption fine spectroscopy (XAFS) revealed a defect-enriched structure (VNi and VO) and low coordination structure (Ni–O and V–O) in NiV-LDH-NS. X-ray absorption spectroscopy (XAS) and electrochemical characterization showed that these higher energy states within Ni and V resulted in intense electronic interactions and fast electron transfer in NiV-LDH-NS; meanwhile, the electron-rich defects accelerated the V4+/V5+ redox, generating hydroxyl radicals (˙OH) to participate in the electrochemical phenol hydroxylation. Analysis by high performance liquid chromatography (HPLC), gas chromatography-mass spectrometry (GC-MS), and 1H nuclear magnetic resonance (1H NMR) further confirmed the existence of target product hydroquinone (HQ), which was optimally achieved with a 72.2% conversion of phenol and a 71.6% selectivity of HQ.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Su Xu,YaNi Yi,HuaYing Li,WeiWei Zhang
Oxytetracycline (OTC), a persistent and poorly biodegradable antibiotic, is increasingly detected in aquatic environments, posing ecological and health risks. Herein, a defect-rich, Co-free MoS₂/PMS system enables ultrafast OTC removal, achieving >99% elimination within 5 min (k obs = 0.791 min⁻¹). The process remained highly efficient across pH 2–10 and in real waters containing natural organic matter and common inorganic ions, demonstrating strong robustness under complex water matrices. Radical-quenching and electron paramagnetic resonance (EPR) analyses confirmed that •OH was the dominant reactive oxygen species (ROS), accompanied by SO₄•⁻ and ¹O₂. X-ray photoelectron spectroscopy (XPS) evidenced Mo⁴⁺/Mo⁶⁺ redox cycling and the participation of surface sulfur species and lattice oxygen, which jointly facilitated PMS activation and ROS generation, thereby establishing a coupled radical-non-radical degradation mechanism. Liquid chromatography–mass spectrometry (LC–MS) identified sequential demethylation, deamination, and ring-opening intermediates, while QSAR-based ecotoxicity assessment indicated an overall decrease in predicted toxicity for most transformation products relative to OTC. Machine-learning analysis (XGBoost with SHAP interpretation) highlighted reaction time, PMS dose, and natural organic matter as the primary determinants of degradation efficiency. Overall, this work integrates a Co-free, light-independent MoS₂/PMS system, refined dual radical–non-radical mechanistic elucidation, comprehensive toxicity mitigation assessment and explainable machine learning, offering both mechanistic and engineering guidance for the sustainable treatment of antibiotic-contaminated wastewater.
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产品关联
DOI
高影响因子
Nano Research
·
2024
·
IF 9.5
Zhang Guiru,Ji Ning,Lyu Shiheng,Ni Baoxin,Shen Peng,Ye Ke,Wang Yuting,Jiang Xuheng,Zhang Hai,Liu Xi,Wang Yongcheng,Jiang Kun
Electrochemically converting CO 2 into value-added chemicals is a promising approach to mitigate anthropogenic carbon emissions, yet largely limited to short-chained C 1 –C 3 products. Herein, we demonstrate a tandem artificial synthesis of biodegradable polyhydroxybutyrate (PHB) plastic from CO 2 building blocks. Batch synthesis of defects-enriched Bi catalyst is firstly demonstrated by plasma bombardment and following in situ electrochemical reduction, which delivers a HCOOH Faradaic efficiency above 80% at tunable concentration from 2 to 250 mM, an energy efficiency up to 41%, and a single-pass carbon conversion efficiency up to 60%. Annular dark field and second electron microscopic analysis, density functional theory (DFT) calcualtions, coupled with H-type and solid-state electrolyzer assessments, point out the vital role of defective and/or stepped Bi surface sites in promoting CO 2 -to-HCOOH conversion. Thereafter, as-synthesized high-purity HCOOH is used as the sole carbon source for C-chain growth within microbial fermentation reactor with Ralstonia eutropha , where activated formate dehydrogenase and increased metabolites related to Calvin–Benson–Bassham cycle are found to be responsible for the enhanced polyester accumulation.
研究领域:
化学工程
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材料科学
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环境科学
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生物化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Fan Zhang,Renjie Ji,Yonghong Liu,Zhijian Li,Zheng Liu,Shuaichen Lu,Yating Wang,Xinlei Wu,Hui Jin,Baoping Cai
Exploring the low-cost and high-efficient electrocatalysts with Pt-like activity for alkaline hydrogen evolution through water splitting is imperative yet challenging. Herein, a simple synthesis combined with electrodeposition and facile electro-oxidation is developed to construct the hollow dendritic self-supported electrode (HDSE). X-ray photoelectron spectroscopy (XPS), X-ray absorption fine structure (XAFS), and electron paramagnetic resonance (EPR) reveal that the surface of HDSE contains the abundant NiO, which is further decorated by fluorine (F)-doped and oxygen vacancies after electro-oxidation process. The resultant HDSE achieves an excellent electrocatalytic performance for hydrogen evolution reaction (HER) in alkaline condition, leading to the extremely low overpotential of 13 mV to drive a current density of −10 mA·cm −2 , and exhibits the long-time stability at the current density of −100 mA·cm −2 and −500 mA·cm −2 , which is superior to the electrocatalytic ability of Pt/C. Density functional theory (DFT) calculations illustrate the NiO modulated by F-doping and oxygen vacancy, could synergistically improve the charge distribution, enhance the conductivity of NiO structure, and optimize the adsorption energy for intermediates of HER, thus accelerating the electrocatalytic ability for hydrogen evolution. This work opens up a new avenue toward the reasonable design of high-efficient and low-cost electrocatalysts for alkaline hydrogen evolution reaction.
研究领域:
材料科学
·
电化学
·
催化
·
可再生能源
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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）