COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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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 .
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高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Wanying Xie,Wei Song,Ji Li,Xiaolei Zhang,Wenyi Dong,Feiyun Sun
Modifying PVDF membrane by blending hydrophilic nano TiO 2 has been highly concerning, but its practical application is not well investigated. In this study, PVDF-TiO 2 membrane was employed in two modes to treat micro-polluted raw water for the first time, direct membrane filtration and pre-oxidation assists membrane filtration. At two filtration modes, the PVDF-TiO 2 membrane had comparable rejection capability to the unmodified PVDF membrane, as the removal of permanganate index (COD Mn ) was 0.26–0.72 mg/L, UV 254 was 0.0070–0.0618 cm −1 , turbidity was 1.60–4.49 NTU, and the total number of colonies was 360–23,780 CFU/mL. As for raw water treatment , using Fe 2+ /sodium dithionite (DTN)/O 2 system as the pre-oxidation process to assist the filtration of the PVDF-TiO 2 membrane was feasible. After optimization, the applicable conditions of the Fe 2+ /DTN/O 2 process were DTN dosage at 100 mg/L and a C Fe / C DTN of 1:4. As a result, the effluent qualities of the PVDF-TiO 2 membrane significantly improved. It was investigated that atrazine (ATZ), COD Mn , UV 254, and turbidity reduced, which was realized by the synergic effects of the pre-oxidation by free radicals and flocculation by iron. Pre-oxidation of the Fe 2+ /DTN/O 2 process could also enhance the permeability of the PVDF-TiO 2 membrane from 53.6 to 58.0 L/(m 2 ·h), nearly two times the PVDF membrane. Besides, the practical fouling of the PVDF-TiO 2 membrane was stably alleviated by the reduced R t , R re, and R ir , mainly due to constraining the internal pore fouling effectively.
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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.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yong Cheng,Han-Qing Zhao,Aqiang Ding,Fei Chen,Jun Liu,Dazhi Fang,Chenglong Li,Yongkui Huang,Peili Lu
The widespread application of quaternary ammonium compounds (QAC) has posed a serious hazard to the environment and human being, and high concentration of Cl − in QAC wastewater may further increase the difficulty of pollutants elimination . In this study, such a QAC wastewater under high salinity conditions was chosen as the target, the prepared Ti/(Ru x Ir y )O 2 anode exhibited favorable catalytic performance for the oxidation and mineralization of QAC under high salinity conditions. Increasing the Ru/Ir ratio of Ti-based electrode coating also slightly promoted the inner catalytic capacity. The combination of electron paramagnetic resonance (EPR) and quenching experiments indicates that 1 O 2 served as a main reactive specie in the Ti/(Ru x Ir y )O 2 electrooxidation system. The increase of pH could decrease the removal efficiency of QAC for the reduced 1 O 2 yield, and the rise of Cl − concentration could favor the QAC oxidation, and Cl − was a better electrolyte to promote the oxidation of organic contaminants when compared to Na 2 SO 4 or Na 2 CO 3 . Additionally, the conversion pathway of the model pollutant was tentatively investigated, the results demonstrated that there were almost no halogenated final products residual by electrocatalytic oxidation with Ti/(Ru x Ir y )O 2 anode. This study not only elucidate the reaction mechanism of Ti/(Ru x Ir y )O 2 anode electrocatalytic oxidation of high salinity QAC wastewater, but also may provide an efficacious and eco-friendly method for the treatment of high salinity QAC wastewater.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
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.
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高影响因子
Nanoscale
·
2023
·
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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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.
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高影响因子
Nanoscale
·
2021
·Vol. 13
·期 16
·7774-7782
·
IF 7.79
Gangyong Li,Guangming Ren,Wei (Alex) Wang,Zongqian Hu
Carbonaceous materials are promising electrode materials for enzymatic biofuel cells (EBFCs) due to their excellent electrical conductivity, chemical and physical stability and biocompatibility. Design and preparation of carbon materials with a hollow structure and a rough surface are of great significance for immobilization of enzymes both inside and outside the carbon materials for EBFC applications. We report herein the synthesis of novel carbonaceous materials consisting of bamboo-shaped hollow N-doped carbon nanotubes (N-CNTs) and C3N4 nanosheets (denoted as N-CNTs@C3N4) as electrode materials for dual-capture of enzymes in glucose/O2 EBFCs. The combination of one-dimensional N-CNTs with an open structure and two-dimensional C3N4 nanosheets forms a three-dimensional crosslinking network that significantly enhances the immobilization of enzymes, electrode stability, and mass transfer of substrates, thus boosting the EBFC performance. As a result, EBFCs equipped with N-CNTs@C3N4 can generate a high open circuit potential of 0.93 V and output a maximum power density of 0.57 mW cm−2 at 0.47 V. Additionally, the as-fabricated glucose/O2 EBFCs are capable of directly harvesting energy from various soft drinks, which indicates the promising applications of the N-CNTs@C3N4 nanocomposite as an electrode material for EBFCs.
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高影响因子
IET Nanobiotechnology
·
2020
·Vol. 14
·期 5
·347-356
·
IF 1.859
Mei Yang,Qingyuan Gui,Jinlei Ma,Lei Qi,Bijun Bao,Yida Huang
In this study, Gd 2 O 2 S:Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) upconversion nanotubes (UCNTs) were synthesised by using Gd(OH) 3 :Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) nanotubes as the template. The luminescent and biological properties of Gd 2 O 2 S:Ln 3+ (Ln 3+ = Yb 3+ , Er 3+ ) UCNTs, along with photodynamic therapy (PDT) applications of the Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 (chlorin e6) nanocomposites, were systematically studied. The resultant UCNTs showed excellent biocompatibility with human retinal pigment cells (ARPE-19) even after a prolonged incubation time of 72 h, and could be used as luminescent probes. Microscopic imaging revealed that the UCNTs existed mainly in cytoplasm. PDT studies on the Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 nanocomposites indicate that the growth of the tumour (cell) could be inhibited dramatically when it was injected (incubated) with Gd 2 O 2 S:8%Yb 3+ , 2%Er 3+ UCNT–Ce6 nanocomposites under the irradiation of 980 nm laser.
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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·24056-24063
·
IF 12.732
Yanfang Chen,Xuemei Yan,Jixiang Xu,Lei Wang
H2O2 has a wide range of uses as an oxidant and is also utilized as a high density and environmentally friendly fuel. In this study, crystalline g-C3N4 was modified with K+, Ni and N-doped carbon by thermal-polymerization of Ni2+-anchored and polyvinyl pyrrolidone-encapsulated melamine-cyanuric acid supramolecules, followed by re-calcination in a KCl–LiCl mixture. The obtained strip-like g-C3N4 nanocrystals exhibited high charge separation efficiency and good light absorption capability. Density-functional theory calculations confirmed that the orbital hybridization of Ni–N atoms enabled the formation of charge-transfer channels, which can capture electrons, achieve enhanced oxygen adsorption and reduction via a two-electron pathway. Under the synergistic effects of K+, Ni and N-doped carbon dopants and crystallinity, the obtained sample exhibited high photocatalytic H2O2 yields of 79.6 μM in O2-saturated pure water, which was 10-fold higher than the yield using pristine g-C3N4. This work provides a novel design for production of highly efficient photocatalysts for H2O2 production.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Bin He,Huanhuan Liu,Zheng Lin,Lei Yan,Jiqiang Ning,Yijun Zhong,Changcheng Zheng,Ziyang Zhang,Yong Hu
The practical application of photocatalytic water splitting is essentially limited by the slow kinetic nature of the water oxidation process. Therefore, it is highly desirable but challenging to explore a low-cost and high-efficiency water oxidation catalyst for the aim of commercialization and industrialization. We herein report the first-time synthesis of a novel and high-efficiency visible-light-driven photocatalyst composed of flower-like Co(CO 3 ) 0.5 (OH)·0.11H 2 O (CCO) nanowires and Bi 2 WO 6 (BWO) nanosheets, i.e. CCO/BWO nanocomposite, via a facile hydrothermal method. Without utilizing any additional cocatalyst, the composite of CCO/BWO in 30% weight ratio exhibits extraordinarily high photoactivity and photostability towards O 2 evolution, achieving an average O 2 generation rate of 953 µmol h −1 g −1 under visible-light irradiation (λ > 420 nm).
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JOURNAL OF POWER SOURCES
·
2012
·
IF 4.951
Jing Lin,Daobin Mu,Ying Jin,Borong Wu,Yunfeng Ma,Feng Wu
Li-rich layered composite Li[Li 0.2 Ni 0.2 Mn 0.6 ]O 2 is prepared by a novel approach in which carbon felt acts as a carrier for synthesis reaction . The as-prepared material is characterized by SEM, ICP and XRD , its electrochemical performance is also examined with galvanostatic charge/discharge and CV measurements. It is showed that the facile process controls effectively the particle growth (in size around 100–200 nm) of the composite and its chemical composition . The as-prepared material shows a high initial discharge capacity about 288 mAh g −1 when charged to 4.8 V, and a retained value of 246.8 mAh g −1 in the 40th cycle. The crystalline structure of the composite is simulated further by Material Studio. It is revealed that the composite has a compatible layer structure merged by Li 2 MnO 3 and LiNi 0.5 Mn 0.5 O 2 , which makes substantial contribution to the cycleability of the electrode. In addition, the lithiation/delithiaion properties including charge transfer resistance and lithium ion diffusion coefficient are studied with electrochemical impedance spectra.
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