ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
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IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
研究领域:
环境科学
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化学工程
·
水处理技术
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DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Jie-wen Liu,Jian Zhang,Ming-jie Xu,Chuan-jin Tian,Xiao-jun Zeng,Chang-an Wang
Developing highly active and reliable Pt-based catalysts is a major challenge for the widespread commercialization of proton-exchange membrane fuel cells. Herein, we have designed Pt3Co@C hollow sphere catalysts by the template method, in which PtCo alloy nanoparticles of approximately 3 nm diameter are anchored in a porous shell of nitrogen-doped carbon hollow spheres. Due to the confinement effect of the porous carbon shell, PtCo alloy nanoparticles possess excellent resistance to sintering, maintaining 2–3 nm size after calcination at 800 °C. Also, Pt3Co@C hollow sphere catalysts exhibit superior catalytic activity and stability in the oxygen reduction reaction, achieving 3.6 times the mass activity of the corresponding commercial Pt/C catalyst. Such catalysts with a mass activity retention rate of 87% after accelerated durability testing and no significant decay in activity after 10,000 potential cycles. Meanwhile, Pt3Co@C catalysts exhibit extremely high catalytic activity and surprising durability for the hydrogen evolution reaction process over the entire pH range. We believe that this methodology provides an insight into the preparation of high-performance electrocatalysts.
研究领域:
材料科学
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电化学
·
催化科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Linfeng Peng,Hang Yin,Lu Zou,Faquan Yu
As a promising energy storage technology, Li-CO 2 /O 2 batteries not only deliver ultrahigh discharge capacity but also capture and convert CO 2 into renewable energy. The exploration into the deposition and decomposition kinetics of discharge product (Li 2 CO 3 ) is urgent for the high thermodynamic stability. Herein, the influence of current density on the essential characteristics of Li 2 CO 3 has been explored. The results show that the Li 2 CO 3 with poor crystallinity and elliptical disk morphology can be obtained at medium current density, corresponding to the excellent electrochemical performance including ultrahigh capacity of 5800 mA h/g, lower discharge-charge gap of 1.15 V, and long-term cycle life of 80 cycles. In addition, the morphology and crystallinity of Li 2 CO 3 are tailored by the relative energy barriers for electron migration and O 2 - generation. At a medium current density (500 mA/g), the accelerated electron migration can realize the nucleation rate equivalent to growth one of Li 2 CO 3 . At this time, Li 2 CO 3 will uniformly deposit on the cathode surface, forming elliptical disk morphology with poor crystallinity. Obviously, this work provides new sights for promoting the development of Li-CO 2 /O 2 battery through rational design of catalysts to accelerate the deposition and decomposition processes of Li 2 CO 3 .
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Xixi Chen,Wanyi Fu,Zhichao Yang,Yulong Yang,Yanjun Li,Hui Huang,Xihui Zhang,Bingcai Pan
Hydrogen peroxide (H 2 O 2 ) is the most commonly used oxidant in advanced oxidation processes for emerging organic contaminant degradation. However, the activation of H 2 O 2 to generate reactive oxygen species is always accompanied by O 2 generation resulting in H 2 O 2 waste. Here, we prepare a Ti doped Mn 3 O 4 /Fe 3 O 4 ternary catalyst (Ti-Mn 3 O 4 /Fe 3 O 4 ) to create abundant oxygen vacancies (OVs), which yields electron delocalization impacts on enhancing the electrical conductivity, accelerating the activation of O 2 to produce H 2 O 2 . In Ti-Mn 3 O 4 /Fe 3 O 4 /H 2 O 2 system, OVs-mediated O 2 /O 2 •− /H 2 O 2 redox cycles trigger the activation of locally generated O 2 , boost the regeneration of O 2 •− and on site produce H 2 O 2 for replenishment. This leads to a 100% removal of tiamulin in 30 min at an unprecedented H 2 O 2 utilization efficiency of 96.0%, which is 24 folds higher than that with Fe 3 O 4 /H 2 O 2 . Importantly, further integration of Ti-Mn 3 O 4 /Fe 3 O 4 catalysts into membrane filtration achieved high rejections of tiamulin (> 83.9%) from real surface water during a continuous 12-h operation, demonstrating broad pH adaptability, excellent catalytic stability and leaching resistance. This work demonstrates a feasible strategy for developing OVs-rich catalysts for improving H 2 O 2 utilization efficiency via activation of locally generated oxygen during the Haber-Weiss reaction.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenqing Hou,Chen Chen,Diya Xie,Yiming Xu
Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH2 (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl4, followed by amination. The solid had a high surface area (828–937 m2/g) and a large pore volume (0.451–0.507 m3/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H2O reduction and oxidation on a film electrode, respectively. However, such a change for H2 evolution in a Na2S/Na2SO3 aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.
研究领域:
材料科学
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化学
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纳米技术
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光化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2023
·
IF 5.7
Yulan Yu,Guanghui Feng,Yujun Jia,Hejun Li
In this work, AlN whisker-reinforced (Zr, Hf)O 2 coating was prepared on SiC coated carbon/carbon composites by sol-gel and plasma spraying methods. Its cyclic ablation resistance was evaluated using an oxyacetylene torch with a heat flux of 2.38 MW/m 2 . After ablation, the coating showed apparently decreased crack sizes and quantity as compared with the one without AlN whisker addition, pointing out its better crack tolerance. Moreover, the coating had a thinner oxidized region based on the linear ablation rate (−0.042 µm/s), greatly lower than that of pure oxide coating (−0.922 µm/s). After detailed observation and characterization, probable protection mechanism was proposed.
研究领域:
材料科学
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航空航天工程
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产品关联
DOI
高影响因子
Small
·
2023
·
IF 13.3
Yuxin Long,Qiang Li,Zidong Zhang,Qingxi Zeng,Dong Liu,Lanling Zhao,Yao Liu,Yebing Li,Yiming Zhang,Kunqian Ji,Zhaorui Zhou,Xue Han,Jun Wang
Li-O 2 batteries could deliver ultra-high theoretical energy density compared to current Li-ion batteries counterpart. The slow cathode reaction kinetics in Li-O 2 batteries, however, limits their electrocatalytic performance. To this end, MoSe 2 and Ni 0.85 Se nanoflakes were decorated in carbon hollow nanoflowers, which were served as the cathode catalysts for Li-O 2 batteries. The hexagonal Ni 0.85 Se and MoSe 2 show good structural compatibility with the same space group, resulting in a stable heterogeneous structure. The synergistic interaction of the unsaturated atoms and the built-in electric fields on the heterogeneous structure exposes abundant catalytically active sites, accelerating ion and charge transport and imparting superior electrochemical activity, including high specific capacities and stable cycling performance. More importantly, the lattice distances of the Ni 0.85 Se (101) plane and MoSe 2 (100) plane at the heterogeneous interfaces are highly matched to that of Li 2 O 2 (100) plane, facilitating epitaxial growth of Li 2 O 2 , as well as the formation and decomposition of discharge products during the cycles. This strategy of employing nonstoichiometric compounds to build heterojunctions and improve Li-O 2 battery performance is expected to be applied to other energy storage or conversion systems.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2023
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IF 6.7
Yingyi Zhang,Lin Zhang,Yuhan Zhang,Rong Ju,Guoqing Wei
Antimicrobial sonodynamic therapy (SDT) has broad application potential in the eradication of multidrug-resistant (MDR) bacterial infections due to its non-invasiveness, absence of resistance concern, and high cytotoxicity. However, the hypoxic infection microenvironment and the rapid depletion of O2 during SDT severely limit the therapeutic efficacy of SDT. Herein, an ultrasound-controllable ROS-responsive nanoplatform (FOT/Fe3O4@Lipo-ICG) was constructed and prepared by encapsulating FOT and Fe3O4 nanoparticles (Fe3O4 NPs) within sonosensitiser ICG-modified liposomes. Both in vitro and in vivo, we observed that the ICG conjugation on the surface of liposomes could effectively maintain a good dispersion and prevent ICG aggregates in complex biological matrices. In addition, the liposomes could significantly block the catalytic activity of the Fe3O4 NPs, as well as the release of FOT, whereas upon US irradiation, the catalytic activity of Fe3O4 NPs was recovered to catalyse the decomposition of endogenous H2O2 into O2 and •OH. Meanwhile, the FOT was successfully released to react with endogenous glutathione to sequentially produce NO. Based on the aforementioned advantages, the FOT/Fe3O4@Lipo-ICG demonstrated potent efficacy in eradicating methicillin-resistant Staphylococcus aureus-induced local infection and sepsis resulting from local infection. Thus, the developed US-controllable nanoplatform offers a promising strategy for enhancing SDT for eradicating MDR bacterial infections.
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Sciences
·
2023
·
IF 6.9
Yi Yuan,Wen-Long Wang,Zhi-Wei Wang,Jin Wang,Qian-Yuan Wu
Carbon nitride has been extensively used as a visible-light photocatalyst, but it has the disadvantages of a low specific surface area, rapid electron–hole recombination, and relatively low light absorbance. In this study, single-atom Ag was successfully anchored on ultrathin carbon nitride (UTCN) via thermal polymerization, the catalyst obtained is called AgUTCN. The Ag hardly changed the carbon nitride's layered and porous physical structure. AgUTCN exhibited efficient visible-light photocatalytic performances in the degradation of various recalcitrant pollutants, eliminations of 85% were achieved by visible-light irradiation for 1 hr. Doping with Ag improved the photocatalytic performance of UTCN by narrowing the forbidden band gap from 2.49 to 2.36 eV and suppressing electron–hole pair recombination. In addition, Ag doping facilitated O 2 adsorption on UTCN by decreasing the adsorption energy from −0.2 to −2.22 eV and favored the formation of O 2 ·− . Electron spin resonance and radical-quenching experiments showed that O 2 ·− was the major reactive species in the degradation of Acetaminophen (paracetamol, APAP).
研究领域:
环境科学
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材料科学
·
化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Yunbo Feng,Qian Wang,Shudong Sun,Weifeng Zhao,Changsheng Zhao
Artificial lung membranes as the core module of the extracorporeal membrane oxygenation technology (ECMO) execute the function of extracorporeal blood-gas barrier accomplishing CO 2 /O 2 exchange with blood. However, the unsatisfactory hemocompatibility and difficulty in functionalization are the prominent challenges faced by current artificial lung membrane materials. In this study, polyethersulfone (PES) composite membranes with self-anticoagulant property and high gas exchange efficient are fabricated by blending PES matrix with poly(vinylamine) (PVAm) modified carboxylic carbon nanotubes (mCNTs) and citrate-based poly(octamethylene-citrate) (POC) pre-polymers. The mCNTs construct specific gas transfer channels within the composite membranes to enhance the gas permeability, while the POC pre-polymers provide anticoagulant property based on the chelation to blood Ca 2+ and the inactivation effect to intrinsic coagulation factors. Importantly, directed by the actual ECMO gas exchange mode, we design a gas-liquid convectional circulation device that could evaluate gas exchange efficiency for the composite membranes under mimetic ECMO state. Therefore, this strategy not only proposes a new design method of advanced artificial lung membranes to solve the practical challenges in the current ECMO technology, but also establishes a scientific testing method to evaluate the gas exchange performance for new-type artificial lung membrane materials in the future.
研究领域:
生物医学工程
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuancheng Qin,Zhenhua Jiang,Yue Guo,Muhammad Asim Mushtaq,Zhen Shen,Wanjun Du,Cailing Ni,Geng Luo,Yu Ji,Zhiqi Zhang,Yonggui Deng,Arshad Hussain,Lasharl Najeeb Ur Rehman,Xingke Cai,Panagiotis Tsiakaras,Jie Zhao
Porous organic polymers (POPs) have emerged as functional materials in photocatalytic degradation of tetracycline (TC) antibiotics but still did not get enough attention on the degradation mechanism and “structure-performance” relationship. It is of great scientific concern to explore the photo-degradation capability of POPs for TC antibiotics under visible light and to reveal their “structure-performance” relationship at the molecular level. Herein, we have constructed a novel benzotriazole-based POP by polymerizing benzotriazole-based structure with melamine. The photo-degradation test results indicate that the POP with benzotriazole-based structure presents an excellent photocatalytic performance with a high TC removal efficiency of 92.12 % and good recyclability. The corresponding pseudo-first-order reaction kinetic constant of benzotriazole-based POP is 6.8 times that of benzene-based one. Such excellent performance of benzotriazole-based POP can be attributed to the physical/chemical property contributions of benzotriazole-based structure to POP, e.g. , the narrow energy bandwidth (2.48 eV) for producing more photo-generated electrons/holes, the small charge transfer resistance for circumventing recombination of photo-generated electrons/holes, and the large number of O 2 − radicals converted from high-activated O 2 that produced by the interactions between photocatalyst and O 2 under visible light irradiation. This strategy of introducing the benzotriazole-based structure into POP opens new avenues to develop next-generation advanced photocatalysts for removing TC antibiotics from wastewater.
研究领域:
环境科学
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材料科学
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光催化技术
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产品关联
DOI
高影响因子
JOURNAL OF ELECTRONIC MATERIALS
·
2023
·Vol. 52
·期 10
·6613-6624
·
IF 2.1
Gong Huixia,Wang Liqin,Wang Jianshe,Liu Qingchao
Lithium-oxygen (Li-O 2 ) batteries have become one of the most promising next-generation energy storage systems due to their high theoretical specific capacity. However, Li-O 2 batteries still face the problem of high charging voltage due to incomplete decomposition of discharge products. Here, a nitrogen-doped hollow spherical carbon composite containing Ni/Co nanoparticles was prepared by hydrothermal and pyrolysis strategies, and used as positive catalyst for Li-O 2 batteries to adjust the morphology of the discharge product. The porous hollow carbon sphere provides sufficient space for the storage of discharge products. Nitrogen-doped carbon nanospheres can change the local charge density, improve the electron transfer performance, and reduce the resistivity of carbon nanospheres. In addition, the abundant M-N x active groups enhance the affinity of the positive electrode to the reaction intermediates, thus regulating the morphology of the discharge product Li 2 O 2 . Benefiting from the above synergistic advantages, the electrochemical performance of the Li-O 2 battery including round-trip efficiency, discharge capacity, and cycling stability is greatly improved. Graphical Abstract
研究领域:
材料科学
·
能源存储技术
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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）