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1.
Gastrointest Endosc ; 2024 Apr 07.
Artículo en Inglés | MEDLINE | ID: mdl-38593933

RESUMEN

BACKGROUND AND AIM: The aim of this study was to investigate the safety and efficacy of appendicoscopy using single-operator cholangioscopy (SOC) for the management of acute obstructive appendicitis. METHODS: We describe 110 cases of acute obstructive appendicitis managed by appendicoscopy between January 2021 and June 2023. The success rate (technical + clinical), procedure time, time to relief abdominal pain using visual analogue scale (VAS), postoperative length of hospital stay, and complications rates were recorded and analyzed. RESULTS: The technical success rate of appendicoscopy was 96.4%; the clinical success rate was 91.8%. The mean procedure time was 20.9±10 minutes (standard deviation [SD]). The abdominal pain score at 6 hours after the procedure was ≤3 (VAS method) in 99.1% of the patients. The average length of postoperative hospital stay was 3.5±1.5 days. No adverse events occurred. CONCLUSION: Appendicoscopy appears to be a feasible and effective alternative therapy for the accurate diagnosis and treatment of acute obstructive appendicitis.

2.
Angew Chem Int Ed Engl ; 63(16): e202400562, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38382041

RESUMEN

Halide solid electrolytes, known for their high ionic conductivity at room temperature and good oxidative stability, face notable challenges in all-solid-state Li-ion batteries (ASSBs), especially with unstable cathode/solid electrolyte (SE) interface and increasing interfacial resistance during cycling. In this work, we have developed an Al3+-doped, cation-disordered epitaxial nanolayer on the LiCoO2 surface by reacting it with an artificially constructed AlPO4 nanoshell; this lithium-deficient layer featuring a rock-salt-like phase effectively suppresses oxidative decomposition of Li3InCl6 electrolyte and stabilizes the cathode/SE interface at 4.5 V. The ASSBs with the halide electrolyte Li3InCl6 and a high-loading LiCoO2 cathode demonstrated high discharge capacity and long cycling life from 3 to 4.5 V. Our findings emphasize the importance of specialized cathode surface modification in preventing SE degradation and achieving stable cycling of halide-based ASSBs at high voltages.

3.
Heliyon ; 10(4): e26009, 2024 Feb 29.
Artículo en Inglés | MEDLINE | ID: mdl-38404797

RESUMEN

Drug delivery systems (DDSs) are designed to deliver drugs to their specific targets to minimize their toxic effects and improve their susceptibility to clearance during targeted transport. Peptides have high affinity, low immunogenicity, simple amino acid composition, and adjustable molecular size; therefore, most peptides can be coupled to drugs via linkers to form peptide-drug conjugates (PDCs) and act as active pro-drugs. PDCs are widely thought to be promising DDSs, given their ability to improve drug bio-compatibility and physiological stability. Peptide-based DDSs are often used to deliver therapeutic substances such as anti-cancer drugs and nucleic acid-based drugs, which not only slow the degradation rate of drugs in vivo but also ensure the drug concentration at the targeted site and prolong the half-life of drugs in vivo. This article provides an profile of the advancements and future development in functional peptide-based DDSs both domestically and internationally in recent years, in the expectation of achieving targeted drug delivery incorporating functional peptides and taking full advantage of synergistic effects.

4.
Small Methods ; 7(7): e2300280, 2023 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-37086111

RESUMEN

Ni-rich layered cathodes with ultrahigh nickel content (≥90%), for example LiNi0.9 Co0.1 O2 (NC0.9), are promising for next-generation high-energy Li-ion batteries (LIBs), but face stability issues related to structural degradation and side reactions during the electrochemical process. Here, surface modulation is demonstrated by integrating a Li+ -conductive nanocoating and gradient lattice doping to stabilize the active cathode efficiently for extended cycles. Briefly, a wet-chemistry process is developed to deposit uniform ZrO(OH)2 nanoshells around Ni0.905 Co0.095 (OH)2 (NC0.9-OH) hydroxide precursors, followed by high temperature lithiation to create reinforced products featuring Zr doping in the crust lattice decorated with Li2 ZrO3 nanoparticles on the surface. It is identified that the Zr4+ infiltration reconstructed the surface lattice into favorable characters such as Li+ deficiency and Ni3+ reduction, which are effective to combat side reactions and suppress phase degradation and crack formation. This surface control is able to achieve an optimized balance between surface stabilization and charge transfer, resulting in an extraordinary capacity retention of 96.6% after 100 cycles at 1 C and an excellent rate capability of 148.8 mA h g-1 at 10 C. This study highlights the critical importance of integrated surface modulation for high stability of cathode materials in next-generation LIBs.

5.
J Am Chem Soc ; 145(13): 7397-7407, 2023 Apr 05.
Artículo en Inglés | MEDLINE | ID: mdl-36961942

RESUMEN

Nickel-rich layered oxides (NLOs) are considered as one of the most promising cathode materials for next-generation high-energy lithium-ion batteries (LIBs), yet their practical applications are currently challenged by the unsatisfactory cyclability and reliability owing to their inherent interfacial and structural instability. Herein, we demonstrate an approach to reverse the unstable nature of NLOs through surface solid reaction, by which the reconstructed surface lattice turns stable and robust against both side reactions and chemophysical breakdown, resulting in improved cycling performance. Specifically, conformal La(OH)3 nanoshells are built with their thicknesses controlled at nanometer accuracy, which act as a Li+ capturer and induce controlled reaction with the NLO surface lattices, thereby transforming the particle crust into an epitaxial layer with localized Ni/Li disordering, where lithium deficiency and nickel stabilization are both achieved by transforming oxidative Ni3+ into stable Ni2+. An optimized balance between surface stabilization and charge transfer is demonstrated by a representative NLO material, namely, LiNi0.83Co0.07Mn0.1O2, whose surface engineering leads to a highly improved capacity retention and excellent rate capability with a strong capability to inhibit the crack of NLO particles. Our study highlights the importance of surface chemistry in determining chemical and structural behaviors and paves a research avenue in controlling the surface lattice for the stabilization of NLOs toward reliable high-energy LIBs.

6.
ACS Appl Mater Interfaces ; 14(28): 32026-32034, 2022 Jul 20.
Artículo en Inglés | MEDLINE | ID: mdl-35793568

RESUMEN

The use of solid-state electrolytes (SSEs) instead of those liquid ones has found promising potential to achieve both high energy density and high safety for their applications in the next-generation energy storage devices. Unfortunately, SSEs also bring forth challenges related to solid-to-solid contact, making the stability of the electrode/electrolyte interface a formidable concern. Herein, using a garnet-type Li6.5La3Zr1.5Ta0.5O12 (LLZT) electrolyte as an example, we demonstrated a facile treatment based on the dip-coating technique, which is highly efficient in modifying the LLZT/Li interface by forming a MgO interlayer. Using polyvinyl pyrrolidone (PVP) as a coordination polymer, uniform and crack-free nanofilms are fabricated on the LLZT pellet with good control of the morphological parameters. We found that the MgO interlayer was highly effective to reduce the interfacial resistance to 6 Ω cm2 as compared to 1652 Ω cm2 of the unmodified interface. The assembled Li symmetrical cell was able to achieve a high critical current density of 1.2 mA cm-2 at room temperature, and it has a long cycling capability for over 4000 h. Using the commercialized materials of LiFePO4 and LiNi0.83Co0.07Mn0.1O2 as the cathode materials, the full cells based on the LLZT@MgO electrolyte showed excellent cyclability and high rate performance at 25 °C. Our study shows the feasibility of precise and controllable surface modification based on a simple liquid phase method and highlights the essential importance of interface control for the future application of high-performance solid-state batteries.

7.
ACS Appl Mater Interfaces ; 14(11): 13379-13387, 2022 Mar 23.
Artículo en Inglés | MEDLINE | ID: mdl-35266694

RESUMEN

The development of potassium-ion batteries (PIBs) is challenged by the shortage of stable cathode materials capable of reversibly hosting the large-sized K+ (1.38 Å), which is prone to cause severe structural degradation and complex phase evolution during the potassiation/depotassiation process. Here, we identified that anionic doping of the layered oxides for PIBs is effective to combat their capacity fading at high voltage (>4.0 V). Taking P2-type K2/3Mn7/9Ni1/9Ti1/9O17/9F1/9 (KMNTOF) as an example, we showed that the partial substitution of O2- by F- enlarged the interlayer distance of the K2/3Mn7/9Ni1/9Ti1/9O2 (KMNTO), which becomes more favorable for fast K+ transition without violent structural destruction. Meanwhile, based on the experimental data and theoretical results, we identified that the introduction of F- anions effectively increased the redox-active Mn cationic concentration by lowering the average valence of the Mn element, accordingly providing more reversible capacity derived from the Mn3+/4+ redox couple, rather than oxygen redox. This anionic doping strategy enables the KMNTOF cathode to deliver a high reversible capacity of 132.5 mAh g-1 with 0.53 K+ reversible (de)intercalation in the structure. We expect that the discovery provides new insights into structural engineering for pursuing stable cathodes to facilitate the future applications of high-performance PIBs.

8.
Small Methods ; 6(5): e2200148, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-35324091

RESUMEN

Layered LiCoO2 (LCO) is one of the most important cathodes for portable electronic products at present and in the foreseeable future. It becomes a continuous push to increase the cutoff voltage of LCO so that a higher capacity can be achieved, for example, a capacity of 220 mAh g-1 at 4.6 V compared to 175 mAh g-1 at 4.45 V, which is unfortunately accompanied by severe capacity degradation due to the much-aggravated side reactions and irreversible phase transitions. Accordingly, strict control on the LCO becomes essential to combat the inherent instability related to the high voltage challenge for their future applications. This review begins with a discussion on the relationship between the crystal structures and electrochemical properties of LCO as well as the failure mechanisms at 4.6 V. Then, recent advances in control strategies for 4.6 V LCO are summarized with focus on both bulk structure and surface properties. One closes this review by presenting the outlook for future efforts on LCO-based lithium ion batteries (LIBs). It is hoped that this work can draw a clear map on the research status of 4.6 V LCO, and also shed light on the future directions of materials design for high energy LIBs.

9.
Chem Commun (Camb) ; 58(10): 1454-1467, 2022 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-35019916

RESUMEN

The increasing demand for high-energy Li-ion batteries (LIBs) continues to push the development of electrode materials, particularly cathode materials, towards their capacity limits. Despite the enormous success, the stability and reliability of LIBs are becoming a serious concern due to the much-aggravated side reactions between electrode materials and organic electrolytes. How to stabilize the cathode/electrolyte interface is therefore an imperative and urgent task drawing considerable attention from both academia and industry. An active treatment on the surface of cathode materials, usually by introducing an inert protection layer, to diminish their side reaction with electrolytes turns out to be a reasonable and effective strategy. This Feature Article firstly outlines our synthesis efforts for the construction of a uniform surface nanocoating on various cathode materials. Different wet chemical routes have been designed to facilitate the control of growth kinetics of targeted coating species so that a precise surface coating could be achieved with nanometer accuracy. Furthermore, we showed the possibility to transform the outer coating layer into a surface doping effect through surface solid reaction at high temperature. A detailed discussion on the structure-performance relationship of these surface-controlled cathode materials is introduced to probe the stabilization mechanism. Finally, perspectives on the development tendency of high-energy cathodes for stable LIBs are provided.

10.
J Am Chem Soc ; 144(5): 2179-2188, 2022 Feb 09.
Artículo en Inglés | MEDLINE | ID: mdl-35080388

RESUMEN

The application of solid-state batteries (SSBs) is challenged by the inherently poor interfacial contact between the solid-state electrolyte (SSE) and the electrodes, typically a metallic lithium anode. Building artificial intermediate nanofilms is effective in tackling this roadblock, but their implementation largely relies on vapor-based techniques such as atomic layer deposition, which are expensive, energy-intensive, and time-consuming due to the monolayer deposited per cycle. Herein, an easy and low-cost wet-chemistry fabrication process is used to engineer the anode/solid electrolyte interface in SSBs with nanoscale precision. This coordination-assisted deposition is initiated with polyacrylate acid as a functional polymer to control the surface reaction, which modulates the distribution and decomposition of metal precursors to reliably form a uniform crack-free and flexible nanofilm of a large variety of metal oxides. For demonstration, artificial Al2O3 interfacial nanofilms were deposited on a ceramic SSE, typically garnet-structured Li6.5La3Zr1.5Ta0.5O12 (LLZT), that led to a significant decrease in the Li/LLZT interfacial resistance (from 2079.5 to 8.4 Ω cm2) as well as extraordinarily long cycle life of the assembled SSBs. This strategy enables the use of a nickel-rich LiNi0.83Co0.07Mn0.1O2 cathode to deliver a reversible capacity of 201.5 mAh g-1 at a considerable loading of 4.8 mg cm-2, featuring performance metrics for an SSB that is competitive with those of traditional Li-ion systems. Our study demonstrates the potential of solution-based routes as an affordable and scalable manufacturing alternative to vapor-based deposition techniques that can accelerate the development of SSBs for practical applications.

11.
Adv Mater ; 33(36): e2100409, 2021 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-34270806

RESUMEN

Due to the obvious advantage in potassium reserves, potassium-ion batteries (PIBs) are now receiving increasing research attention as an alternative energy storage system for lithium-ion batteries (LIBs). Unfortunately, the large size of K+ makes it a challenging task to identify suitable electrode materials, particularly cathode ones that determine the energy density of PIBs, capable of tolerating the serious structural deformation during the continuous intercalation/deintercalation of K+ . It is therefore of paramount importance that proper design principles of cathode materials be followed to ensure stable electrochemical performance if a practical application of PIBs is expected. Herein, the current knowledge on the structural engineering of cathode materials acquired during the battle against its performance degradation is summarized. The K+ storage behavior of different types of cathodes is discussed in detail and the structure-performance relationship of materials sensitive to their different lattice frameworks is highlighted. The key issues facing the future development of different categories of cathode materials are also highlighted and perspectives for potential approaches and strategies to promote the further development of PIBs are provided.

12.
Medicine (Baltimore) ; 100(25): e26405, 2021 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-34160426

RESUMEN

BACKGROUND: When a person feels dental pain, it brings great discomfort and damages the quality of life. Symptomatic apical periodontitis is identified as the most frequent cause that triggers dental pain. Symptomatic apical periodontitis arises from an infection or inflammation in the pulpless root canal structure. According to clinical guidelines, the primary form of therapy for such teeth entails removing the inflammation or infection source through local surgical procedures. Presently, systemic antibiotics are recommended only for cases where there is clear indication of an infectious spread or a systemic involvement. Therefore, this study aims to assess the efficacy and level of safety of using antibiotics to treat adult symptomatic apical periodontitis patients. METHODS: The present protocol study will conduct a search on electronic databases to look for randomized controlled trials (RCTs) that have evaluated the effectiveness and safety of antibiotics when used to treat adult patients with symptomatic apical periodontitis. The databases will be search from their beginning to April 2021. The search is not bound by publication status or language restrictions. The following databases will be searched: Web of Science, PubMed, the Cochrane Library, Chinese National Knowledge Infrastructure, and EMBASE. This study will employ ZETOC Conference Proceedings and OpenGrey to identify potential grey literature. Afterwards, 2 independent authors will select the studies, extract data from the studies, and conduct a risk assessment to check for bias. All discrepancies between the authors will be resolute via discussion involving a third independent author. The data synthesis and statistical analysis of this study will be done with the RevMan software (Version: 5.3). RESULTS: The present protocol report will provide high-quality evidence related to the efficacy and level of safety when using antibiotics to treat mature symptomatic apical periodontitis patients. CONCLUSION: The outcomes of the present study will update the evidence available for assessing the efficacy and safeness of using antibiotics to treat mature symptomatic apical periodontitis patients. ETHICS AND DISSEMINATION: This study does not require an ethical approval since individual patient data is not included in any form. REGISTRATION NUMBER: DOI 10.17605/OSF.IO/CVP8 M (https://osf.io/cvp8m/).


Asunto(s)
Antibacterianos/administración & dosificación , Periodontitis Crónica/tratamiento farmacológico , Periodontitis Periapical/tratamiento farmacológico , Odontalgia/tratamiento farmacológico , Adulto , Antibacterianos/efectos adversos , Periodontitis Crónica/complicaciones , Periodontitis Crónica/diagnóstico , Periodontitis Crónica/psicología , Humanos , Metaanálisis como Asunto , Periodontitis Periapical/complicaciones , Periodontitis Periapical/diagnóstico , Periodontitis Periapical/psicología , Calidad de Vida , Ensayos Clínicos Controlados Aleatorios como Asunto , Revisiones Sistemáticas como Asunto , Odontalgia/etiología , Odontalgia/psicología , Resultado del Tratamiento
13.
Acc Chem Res ; 54(1): 221-231, 2021 01 05.
Artículo en Inglés | MEDLINE | ID: mdl-33284018

RESUMEN

Hollow carbon-based nanospheres (HCNs) have been demonstrated to show promising potential in a large variety of research fields, particularly electrochemical devices for energy conversion/storage. The current synthetic protocols for HCNs largely rely on template-based routes (TBRs), which are conceptually straightforward in creating hollow structures but challenged by the time-consuming operations with a low yield in product as well as serious environmental concerns caused by hazardous etching agents. Meanwhile, they showed inadequate ability to build complex carbon-related architectures. Innovative strategies for HCNs free from extra templates thus are highly desirable and are expected to not only ensure precise control of the key structural parameters of hollow architectures with designated functionalities, but also be environmentally benign and scalable approaches suited for their practical applications.In this Account, we outline our recent research progress on the development of template-free protocols for the creation of HCNs with a focus on the acquired mechanical insight into the hollowing mechanism when no extra templates were involved. We demonstrated that carbon-based particles themselves could act as versatile platforms to create hollow architectures through an effective modulation of their inner chemistry. By means of reaction control, the precursor particles were synthesized into solid ones with a well-designed inhomogeneity inside in the form of different chemical parameters such as molecular weight, crystallization degree, and chemical reactivity, by which we not only can create hollow structures inside particles but also have the ability to tune the key features including compositions, porosity, and dimensional architectures. Accordingly, the functionalities of the prepared HCNs could be systematically altered or optimized for their applications. Importantly, the discussed synthesis approaches are facile and environmentally benign processes with potential for scale-up production.The nanoengineering of HNCs is found to be of special importance for their application in a large variety of electrochemical energy storage and conversion systems where the charge transfer and structural stability become a serious concern. Particular attention in this Account is therefore directed to the potential of HCNs in battery systems such as sodium ion batteries (NIBs) and potassium ion batteries (KIBs), whose electrochemical performances are plagued by the destructive volumetric deformation and sluggish charge diffusion during the intercalation/deintercalation of large-size Na+ or K+. We demonstrated that precise control of the multidimensional factors of the HCNs is critical to offer an optimized design of sufficient reactive sites, excellent charge and mass transport kinetics, and resilient electrode structure and also provide a model system suitable for the study of complicated metal-ion storage mechanisms, such as Na+ storage in a hard carbon anode. We expect that this Account will spark new endeavors in the development of HCNs for various applications including energy conversion and storage, catalysis, biomedicine, and adsorption.

14.
Nanoscale ; 11(42): 20284-20294, 2019 Nov 14.
Artículo en Inglés | MEDLINE | ID: mdl-31633137

RESUMEN

Molybdenum disulfide (MoS2) is a potential earth-abundant electrocatalyst for the hydrogen evolution reaction (HER), but the lack of in-depth understanding of its intrinsic activity still impedes the further optimization and design of MoS2-based electrocatalysts. Herein, we report a facile in situ hydrothermal synthetic method to prepare vertical MoxSy arrays grown on guar gum-derived carbon aerogels (GCA), termed MoxSy@GCA. The obtained well-assembled MoxSy@GCA architectures consist of uniform, few-layered and S-edge-rich MoxSy nanoflakes with a length of approximately 100 nm, which effectively prevent the inherent stacking among MoxSy layers and connect the charge transfer path between interlayers, thus endowing MoxSy@GCA with a huge number of active sites and high conductivity. Benefitting from all these advantages, the optimal Mo4S16@GCA exhibited extraordinary HER/OER performances, including a low onset potential for both the HER (24.28 mV) and OER (1.53 V), and a low overpotential at 10 mA cm-2 for the HER (54.13 mV) and OER (370 mV), which are both extremely close to that of the noble Pt/C. Furthermore, a series of operando Raman spectroscopy measurements on Mo4S16@GCA were conducted to identify the intrinsic HER/OER-active sites during the HER and OER process. The results show that the S-H bond is generated simultaneously as HER/OER excitation, indicating the rich S-edge may be the intrinsic active site, which will accelerate the HER/OER kinetic process. Density functional theory (DFT) calculations revealed that the observed superb HER/OER activity can be attributed to the synergistic effect of rich S-edge of MoxSy and confinement effect of GCA, which collaboratively promote the proton adsorption and electrocatalytic kinetics. Reasonably, this study will have profound guiding value for the rational tailoring of the microstructure and size of transition metal electrocatalysts via hierarchical porous carbon aerogels.

15.
Nat Commun ; 9(1): 648, 2018 02 08.
Artículo en Inglés | MEDLINE | ID: mdl-29422617

RESUMEN

The original HTML version of this Article omitted to list Yeshayahu Lifshitz as a corresponding author and incorrectly listed Shuit-Tong Lee as a corresponding author.Correspondingly, the original PDF version of this Article incorrectly stated that "Correspondence and requests for materials should be addressed to X.J. (email: xin.jiang@uni-siegen.de), or to Y.L. (email: yangl@suda.edu.cn), or to S.-T.L. (email: shayli@technion.ac.il), or to Z.K. (email: zhkang@suda.edu.cn)", instead of the correct "Correspondence and requests for materials should be addressed to X.J. (email: xin.jiang@uni-siegen.de), or to Y. Liu (email: yangl@suda.edu.cn), or to Y. Lifshitz (email: shayli@technion.ac.il), or to Z.K. (email: zhkang@suda.edu.cn)".This has now been corrected in the PDF and HTML versions of the Article.

16.
Nat Commun ; 8(1): 1828, 2017 11 28.
Artículo en Inglés | MEDLINE | ID: mdl-29184053

RESUMEN

Syngas, a CO and H2 mixture mostly generated from non-renewable fossil fuels, is an essential feedstock for production of liquid fuels. Electrochemical reduction of CO2 and H+/H2O is an alternative renewable route to produce syngas. Here we introduce the concept of coupling a hydrogen evolution reaction (HER) catalyst with a CDots/C3N4 composite (a CO2 reduction catalyst) to achieve a cheap, stable, selective and efficient route for tunable syngas production. Co3O4, MoS2, Au and Pt serve as the HER component. The Co3O4-CDots-C3N4 electrocatalyst is found to be the most efficient among the combinations studied. The H2/CO ratio of the produced syngas is tunable from 0.07:1 to 4:1 by controlling the potential. This catalyst is highly stable for syngas generation (over 100 h) with no other products besides CO and H2. Insight into the mechanisms balancing between CO2 reduction and H2 evolution when applying the HER-CDots-C3N4 catalyst concept is provided.

17.
Adv Mater ; 29(32)2017 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-28640515

RESUMEN

Self-healing is the way by which nature repairs damage and prolongs the life of bio entities. A variety of practical applications require self-healing materials in general and self-healing polymers in particular. Different (complex) methods provide the rebonding of broken bonds, suppressing crack, or local damage propagation. Here, a simple, versatile, and cost-effective methodology is reported for initiating healing in bulk polymers and self-healing and anticorrosion properties in polymer coatings: introduction of carbon dots (CDs), 5 nm sized carbon nanocrystallites, into the polymer matrix forming a composite. The CDs are blended into polymethacrylate, polyurethane, and other common polymers. The healing/self-healing process is initiated by interfacial bonding (covalent, hydrogen, and van der Waals bonding) between the CDs and the polymer matrix and can be optimized by modifying the functional groups which terminate the CDs. The healing properties of the bulk polymer-CD composites are evaluated by comparing the tensile strength of pristine (bulk and coatings) composites to those of fractured composites that are healed and by following the self-healing of scratches intentionally introduced to polymer-CD composite coatings. The composite coatings not only possess self-healing properties but also have superior anticorrosion properties compared to those of the pure polymer coatings.

18.
ACS Appl Mater Interfaces ; 9(24): 20585-20593, 2017 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-28569511

RESUMEN

Hydrogen production by photocatalytic overall water-splitting represents an ideal pathway for clean energy harvesting, for which developing high-efficiency catalysts has been the central scientific topic. Nanosized CoO with high solar-to-hydrogen efficiency (5%) is one of the most promising catalyst candidates. However, poor understanding of this photocatalyst leaves the key issue of rapid deactivation unclear and severely hinders its wide application. Here, we report a sub-micrometer CoO octahedron photocatalyst with high overall-water-splitting activity and outstanding ability of H2O2-resistance poisoning. We show that the deactivation of CoO catalyst originates from the unintended thermoinduced oxidation of CoO during photocatalysis, with coexistence of oxygen and water. We then demonstrate that introduction of graphene, as a heat conductor, largely enhanced the photocatalytic activity and stability of the CoO. Our work not only provides a new insight of CoO for photocatalytic water splitting but also demonstrates a new concept for photocatalyst design.

19.
Nanoscale ; 9(1): 298-304, 2017 Jan 07.
Artículo en Inglés | MEDLINE | ID: mdl-27910981

RESUMEN

Electrochemical reduction of CO2 is a key component of many prospective artificial technologies for renewable carbon-containing fuels, but it still suffers from the high overpotentials required to drive the process, low selectivity for diversiform products and the high cost of the catalyst. Here, we report that Cu-CDots nanocorals is a highly efficient, low-cost and stable electrocatalyst for CO2 reduction in aqueous solution. The major product of CO2 reduction on the Cu-CDots nanocorals is HCOOH with an inconceivable low overpotential of 0.13 V and a high Faraday efficiency of 79% at a moderate potential of -0.7 V vs. RHE. In the present system, CDots can increase the adsorption capacity of CO2 molecules and H+, which play important roles in CO2 reduction. The high selectivity of HCOOH for CO2 reduction may be ascribed to that CDots can greatly diminish the HCOOH desorption energy and improve the catalytic selectivity for HCOOH. Furthermore, Cu-CDots nanocorals exhibit a long-term stability during 5 h-electrolysis.

20.
Nanoscale ; 8(39): 17314-17321, 2016 Oct 06.
Artículo en Inglés | MEDLINE | ID: mdl-27714093

RESUMEN

Carbon dot and BiVO4 quantum dot composites (CDs/BiVO4 QDs) show a significantly improved photocatalytic activity and high stability for overall water splitting. By using 5% CDs/BiVO4 QDs as photocatalysts, the H2 evolution of 0.92 µmol h-1, was achieved under solar light irradiation without any cocatalysts or sacrificial reagents, which is about 4 times that of BiVO4 QDs (0.21 µmol h-1). Note that, for the CD/BiVO4 QD catalyst, the produced H2 and O2 are approximately equal to the stoichiometric ratio (H2 : O2 = 1.80 : 1), while that of BiVO4 QDs is nonstoichiometric (about only 0.06 : 1). In addition, the present water splitting occurs via a two-electron pathway and CDs and BiVO4 QDs served as the reduction and oxidation reaction active sites, respectively.

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