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1.
Nano Lett ; 24(39): 12095-12101, 2024 Oct 02.
Article in English | MEDLINE | ID: mdl-39291849

ABSTRACT

Aqueous calcium ion batteries, promising for energy storage, are still challenged by very limited anode choices. Although a Zn metal anode is popular in aqueous batteries, interface instability due to incessant corrosion and severe Zn dendrites hinders its development. Here, an interphase layer with densely packed nanocrystals of Ca3(CO3)2(OH)2·1.5H2O and ZnF2, and amorphous organic species, is demonstrated for a Zn metal anode with 1 M calcium trifluoromethyl sulfonate aqueous electrolyte. The hybrid interface fully avoids direct Zn-H2O contact, maintains fast ion conductivity, and effectively prevents corrosion and dendrite growth. Therefore, the symmetric cell stably lasts for 1600 h at 0.5 mA cm-2 and 2.5 mAh cm-2, far superior to 150 h for the control cell. Furthermore, the device maintains 80% capacity retention after 700 cycles at 1 A g-1, outperforming 13% retention after 200 cycles for the control device. This work indicates that interface and interphase engineering is also crucial for aqueous batteries.

2.
J Am Chem Soc ; 146(26): 17784-17792, 2024 Jul 03.
Article in English | MEDLINE | ID: mdl-38916273

ABSTRACT

Well-established knowledge about inversion-symmetric Bi2TexSe3-x topological insulators characterizes the promising new-generation quantum device. Noticeably, the inversion asymmetric phase containing different surface electronic structures may create an extra topological phenomenon pointing to a new device paradigm. Herein, Janus Bi2TeSe2 single-crystal nanosheets with an unconventional stacking sequence of Se-Bi-Se-Bi-Te are realized via chemical vapor deposition growth, which is clarified by atomically resolved AC-STEM and elemental mapping. An obvious polarization-dependent second-harmonic generation with a representative 6-fold rotational symmetry is detected due to the broken out-of-plane mirror symmetry in this system. Low-temperature transport measurements display a strange metal-like linear-in-temperature resistivity. Anomalous conductance peaks under low magnetic fields induced by the weak antilocalization effect of topological surface states and the two-dimensional transport-dominated anisotropic magnetoresistance are revealed. These findings correlate the Janus Bi2TeSe2 phase with emerging physics topics, which would inspire fresh thoughts in well-developed Bi3TexSe3-x topological insulators and open up opportunities for exploring hybrid nonlinear optoelectronic topological devices.

3.
Small ; 20(1): e2305161, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37641192

ABSTRACT

Single-atom catalysts (SACs) are promising cathode materials for addressing issues faced by lithium-sulfur batteries. Considering the ample chemical space of SACs, high-throughput calculations are efficient strategies for their rational design. However, the high throughput calculations are impeded by the time-consuming determination of the decomposition barrier (Eb ) of Li2 S. In this study, the effects of bond formation and breakage on the kinetics of SAC-catalyzed Li2 S decomposition with g-C3 N4 as the substrate are clarified. Furthermore, a new efficient and easily-obtained descriptor Li─S─Li angle (ALi─S─Li ) of adsorbed Li2 S, different from the widely accepted thermodynamic data for predicting Eb , which breaks the well-known Brønsted-Evans-Polanyi relationship, is identified. Under the guidance of ALi─S─Li , several superior SACs with d- and p-block metal centers supported by g-C3 N4 are screened to accelerate the sulfur redox reaction and fix the soluble lithium polysulfides. The newly identified descriptor of ALi─S─Li can be extended to rationally design SACs for Na─S batteries. This study opens a new pathway for tuning the performance of SACs to catalyze the decomposition of X2 S (X = Li, Na, and K) and thus accelerate the design of SACs for alkaline-chalcogenide batteries.

4.
Phys Chem Chem Phys ; 26(7): 5858-5867, 2024 Feb 14.
Article in English | MEDLINE | ID: mdl-38305023

ABSTRACT

Lithium-sulfur (Li-S) batteries are considered as one of the promising next-generation energy storage devices due to their characteristics of high energy density and low cost. However, the shuttle effect and sluggish conversion of lithium polysulfide (LiPs) have hindered their commercial applications. To address these issues, in our previous works, we have screened several highly efficient single atom catalysts (SACs) (MN4@G, M = V, Mo and W) with atomically dispersed transition metal atoms supported by nitrogen doped graphene based on high throughput calculations. Nevertheless, they still suffer from low loading of metal centers and unsatisfactory capability for accelerating the reaction kinetics. To tackle such problems, based on first-principles calculations, we systematically investigated the heterointerface effect on the catalytic performance of such three MN4@G toward sulfur conversion upon forming heterostructures with 5 typical two-dimensional materials of TiS2, C3N4, BN, graphene and reduced graphene oxide. Guided by efficient descriptors proposed in our previous work, we screened VN4@G/TiS2, MoN4@G/TiS2 and WN4@G/TiS2 possessing low Li2S decomposition barriers of 0.54, 0.44 and 0.41 eV, respectively. They also possess enhanced capabilities for catalyzing the sulfur reduction reaction as well as stabilizing soluble LiPs. More interestingly, the heterointerface can enhance the capability of the carbon atoms far away from the metal centers for trapping LiPs. This work shows that introducing a heterointerface is a promising strategy to boost the performance of SACs in Li-S batteries.

5.
BMC Geriatr ; 24(1): 790, 2024 Sep 28.
Article in English | MEDLINE | ID: mdl-39342216

ABSTRACT

BACKGROUND: Myceliophthora heterothallica belonging to Myceliophthora is considered as an environmental fungus and has not been reported to be pathogenic or colonizing in recent literature. The present case firstly reports a ventilation-associated pneumonia caused by Myceliophthora heterothallica among the aged adult. CASE PRESENTATION: A 67-years-old Asian female patient suffering from a sudden disturbance of consciousness for 3 h was admitted to our hospital. Cardiac arrest occurred during emergency transport, and sinus rhythm was restored after cardiopulmonary resuscitation. Invasive mechanical ventilation was given to this patient for respiratory failure. After mechanical ventilation, the lung CT images showed multiple cuneiform nodules arranging subpleural accompanying with ground-glass opacity. On the 5th day of mechanical ventilation, Myceliophthora heterothallica was cultured from endotracheal aspirates. Two methods, namely automatic microbial identification system and internal transcribed spacer sequencing were employed to identify this fungus. The present case firstly uncovered the colonization ability and pathogenicity of Myceliophthora heterothallica in the respiratory tract. After 28d of treatment with piperacillin-tazobactam, this patient weaned from the ventilator and recovered from consciousness with lung infection disappearance. CONCLUSIONS: This is the first case report of ventilation-associated pneumonia in the aged patient caused by Myceliophthora heterothallica. This current case is worth for the clinical diagnosis and treatment of Myceliophthora heterothallica infection, and also enriches new pathogenic species found of thermothelomyces species.


Subject(s)
Pneumonia, Ventilator-Associated , Sordariales , Aged , Female , Humans , Pneumonia, Ventilator-Associated/microbiology , Pneumonia, Ventilator-Associated/diagnosis , Sordariales/pathogenicity , Opportunistic Infections/diagnosis , Opportunistic Infections/microbiology
6.
Eur Child Adolesc Psychiatry ; 33(4): 1017-1028, 2024 Apr.
Article in English | MEDLINE | ID: mdl-37166521

ABSTRACT

The present study measured serum levels of vitamin A (VA) and vitamin D (VD) in children with chronic tic disorders (CTD) and investigated their potential association with CTD and comorbidity of attention deficit hyperactivity disorder (ADHD) and the association of their co-insufficiencies or deficiencies with CTD symptoms. A total of 176 children (131 boys and 45 girls, median age of 9 years) with CTD were recruited as the CTD group. During the same period, 154 healthy children were selected as the healthy control (HC) cohort. Circulating retinol and 25-hydroxyvitamin D (25[OH]D) levels were measured for all participants using high-performance liquid chromatography (HPLC) and tandem mass spectrometry. The Yale Global Tic Severity Scale (YGTSS) was employed for the assessment of tic status and CTD impairment. The Swanson, Nolan, and Pelham Rating Scale (SNAP-IV) and the Children's Yale-Brown Obsessive-Compulsive Scale (CY-BOCS) were used to evaluate comorbidity symptoms. CTD pediatric participants exhibited markedly diminished circulating retinol and 25(OH)D levels compared to HCs. Moreover, VA and VD deficiencies and their co-insufficiencies/deficiencies were more prevalent in CTD participants than HCs. Circulating 25(OH)D levels were inversely proportional to the YGTSS motor tic scores. YGTSS scores in CTD children with only VA or VD insufficiency or deficiency or with VA and VD co-insufficiency/deficiency did not differ from those in CTD children with normal VA and VD. CTD children with comorbid ADHD displayed reduced circulating retinol and 25(OH)D concentrations and elevated prevalence of VD deficiency compared to CTD participants without comorbid ADHD. Lower serum retinol content was intricately linked to the presence of elevated CTD and comorbid ADHD. VA and VD deficiencies and their co-insufficiencies/deficiencies were markedly enhanced in CTD pediatric participants compared to HCs. Lower VA concentration was linked to the presence of enhanced CTD and comorbid ADHD. Therefore, children with CTD, especially with comorbid ADHD, may be at a higher risk of VA or VD deficiency, which may prompt the clinicians to consider whether blood tests for VA and VD in CTD children would be helpful for clinical care.

7.
Nano Lett ; 23(24): 11742-11748, 2023 Dec 27.
Article in English | MEDLINE | ID: mdl-38064584

ABSTRACT

Two-dimensional (2D) materials with exotic transport behaviors have attracted extensive interest in microelectronics and condensed matter physics, while scaled-up 2D thin films compatible with the efficient wet-chemical etching process represent realistic advancement toward new-generation integrated functional devices. Here, thickness-controllable growth and chemical patterning of high-quality Bi2O2Te continuous films are demonstrated. Noticeably, except for an ultrahigh mobility (∼45074 cm2 V-1 s-1 at 2 K) and obvious Shubnikov-de Hass quantum oscillations, a 2D transport channel and large linear magnetoresistance are revealed in the patterned Bi2O2Te films. Investigation implies that the linear magnetoresistance correlates with the inhomogeneity described by P. B. Littlewood's theory and EMT-RRN theory developed recently. These results not only reveal the nonsaturating linear magnetoresistance in high-quality Bi2O2Te but shed light on understanding the corresponding physical origin of linear magnetoresistance in 2D high-mobility semiconductors and providing a pathway for the potential application in multifunctional electronic devices.

8.
Angew Chem Int Ed Engl ; 63(36): e202408758, 2024 Sep 02.
Article in English | MEDLINE | ID: mdl-38899532

ABSTRACT

Electrochemical nitrate reduction reaction (NitRR) uses nitrate from wastewater, offering a hopeful solution for environmental issues and ammonia production. Yet, varying nitrate levels in real wastewater greatly affect NitRR, slowing down its multi-step process. Herein, a multi-strategy approach was explored through the design of ordered mesoporous intermetallic AuCu3 nanocorals with ultrathin Au skin (meso-i-AuCu3@ultra-Au) as an efficient and concentration-versatile catalyst for NitRR. The highly penetrated structure, coupled with the compressive stress exerted on the skin layer, not only facilitates rapid electron/mass transfer, but also effectively modulates the surface electronic structure, addressing the concentration-dependent challenges encountered in practical NitRR process. As expected, the novel catalyst demonstrates outstanding NitRR activities and Faradaic efficiencies exceeding 95 % across a real and widespread concentration range (10-2000 mM). Notably, its performance at each concentration matched or exceeded that of the best-known catalyst designed for that concentration. Multiple operando spectroscopies unveiled the catalyst concurrently optimized the adsorption behavior of different intermediates (adsorbed *NOx and *H) while expediting the hydrogenation steps, leading to an efficient overall reduction process. Moreover, the catalyst also displays promising potential for use in ammonia production at industrial-relevant current densities and in conceptual zinc-nitrate batteries, serving trifunctional nitrate conversion, ammonia synthesis and power supply.

9.
Angew Chem Int Ed Engl ; 63(28): e202405798, 2024 Jul 08.
Article in English | MEDLINE | ID: mdl-38659324

ABSTRACT

RuO2 has been considered as the most likely acidic oxygen evolution reaction (OER) catalyst to replace IrO2, but its performance, especially long-term stability under harsh acidic conditions, is still unacceptable. Here, we propose a grain boundary (GB) engineering strategy by fabricating the ultrathin porous RuO2 nanosheet with abundant of grain boundaries (GB-RuO2) as an efficient acid OER catalyst. The involvement of GB induces significant tensile stress and creates an unsaturated coordination environment, effectively optimizing the adsorption of intermediates and stabilizing active site structure during OER process. Notably, the GB-RuO2 not only exhibits a low overpotential (η10=187 mV) with an ultra-low Tafel slope (34.5 mV dec-1), but also steadily operates for over 550 h in 0.1 M HClO4. Quasi in situ/operando methods confirm that the improved stability is attributed to GB preventing Ru dissolution and greatly inhibiting the lattice oxygen oxidation mechanism (LOM). A proton exchange membrane water electrolysis (PEMWE) using the GB-RuO2 catalyst operates a low voltage of 1.669 V at 2 A cm-2 and operates stably for 100 h at 100 mA cm-2.

10.
J Am Chem Soc ; 145(38): 20975-20984, 2023 Sep 27.
Article in English | MEDLINE | ID: mdl-37703097

ABSTRACT

The progress of unconventional superconductors at the two-dimensional (2D) limit has inspired much interest. Recently, a new superconducting system was discovered in the semimetallic ternary Bi-O-S family. However, pure-phase crystals are difficult to synthesize because of the complicated stacking sequence of multiple charged layers and similar formation kinetics among ternary polytypes, leaving several fundamental issues regarding the structure-superconductivity correlation unresolved. Herein, 2D single-crystal ultrathin Bi3O2S3 nanosheets are prepared by using low-pressure chemical vapor deposition, and their atomic arrangement is clarified. Magnetotransport measurements indicate a superconducting transition at ∼6.1 K that is thickness-independent. The transport results demonstrate 2D superconducting characteristics, such as the Berezinskii-Kosterlitz-Thouless transition, and strong anisotropy with magnetic field orientations following the 2D Tinkham formula. The difference from superconductivity of powder is demonstrated from the perspective of their corresponding microstructures. These results corroborate the superconducting behavior of Bi3O2S3, providing fresh insights into the search for other bismuth oxychalcogenides and derivative BiS2-based analogues at the 2D limit.

11.
Small ; 19(39): e2301005, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37246249

ABSTRACT

Electrolyte engineering is a feasible strategy to realize high energy density lithium metal batteries. However, stabilizing both lithium metal anodes and nickel-rich layered cathodes is extremely challenging. To break through this bottleneck, a dual-additives electrolyte containing fluoroethylene carbonate (10 vol.%) and 1-methoxy-2-propylamine (1 vol.%) in conventional LiPF6 -containing carbonate-based electrolyte is reported. The two additives can polymerize and thus generate dense and uniform LiF and Li3 N-containing interphases on both electrodes' surfaces. Such robust ionic conductive interphases not only prevent lithium dendrite formation in lithium metal anode but also suppress stress-corrosion cracking and phase transformation in nickel-rich layered cathode. The advanced electrolyte enables Li||LiNi0.8 Co0.1 Mn0.1 O2 stably cycle for 80 cycles at 60 mA g-1 with a specific discharge capacity retention of 91.2% under harsh conditions.

12.
Phys Chem Chem Phys ; 25(37): 25761-25771, 2023 Sep 27.
Article in English | MEDLINE | ID: mdl-37724050

ABSTRACT

Electrocatalysis is involved in many energy storage and conversion devices, triggering research and development of electrocatalysts, particularly single-atom catalysts (SACs). The introduction of the strain effect to enhance the performance of SACs has drawn ever-increasing research attention, which can tailor the local atomic and electronic structure of active sites. Herein, via high throughput calculations, we have explored the effects of strain on the catalytic performance of SACs with MN4 configuration for electrochemical reactions of N2 and O2 by incorporating d- and p-block single metal atoms into BN nanocages (BNNCs). The calculations demonstrate that Os@BNNC exhibits the highest catalytic activity for the nitrogen reduction reaction (NRR) with a limiting potential of -0.29 V. Co@BNNC can serve as an excellent bifunctional SAC for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), with overpotentials of 0.32 and 0.37 V, respectively. In particular, Sn@BNNC with a p-block metal as the active center is a competitive SAC for the ORR with an overpotential of 0.64 V. More interestingly, the NRR and ORR performances of SACs supported by BNNCs have a close correlation with the structural and electronic properties of adsorbed N2 and O2 molecules, which proves that controlling the adsorption energy of N2 and O2 molecules is crucial to improving the catalytic activity of BNNC. The current investigation opens up an avenue for designing SACs embedded in nanocages possessing intrinsically curved surfaces for electrochemical reactions.

13.
Sensors (Basel) ; 23(10)2023 May 17.
Article in English | MEDLINE | ID: mdl-37430740

ABSTRACT

The electrical performance of the feed array is degraded because of the position deviation of the array elements caused by manufacturing and processing, which cannot meet the high performance feeding requirements of large feed arrays. In this paper, a radiation field model of the helical antenna array considering the position deviation of array elements is proposed to investigate the influence law of position deviation on the electrical performance of the feed array. With the established model, the rectangular planar array and the circular array of the helical antenna with a radiating cup are discussed and the relationship between electrical performance index and position deviation is established by numerical analysis and curve fitting method. The research results show that the position deviation of the antenna array elements will lead to the rise of the sidelobe level, the deviation of the beam pointing, and the increase of the return loss. The valuable simulation results provided by this work can be used in antenna engineering, guiding antenna designers to set optimal parameters when fabricating antennae.

14.
Nano Lett ; 22(24): 9951-9957, 2022 Dec 28.
Article in English | MEDLINE | ID: mdl-36512484

ABSTRACT

Bending/tension mechanics is one of the core issues for nanowires in flexible free-standing transport and sensor applications, but it remains a challenge to tailor the mechanical performance beyond the inherent properties. Herein, based on structure engineering, silicon-based Mn5Si3@SiO2 nanocables are proposed and demonstrated as versatile nanosystems. Except for outstanding toughness, large ultimate strain, and great strength, they display diverse mechanical behaviors such as simplex elasticity, plasticity, and viscoelasticity under different external conditions. The tunable performances originate from synergetic effects between the core and shell components, like the atomic bonding transitional interface and space confinement, which induce optimizing internal stress distribution and the dislocation evolution mechanism in the core. The related mechanical performance is revealed carefully. The bending and tension dynamic picture, quantitative force curve, stress-strain dependence, and the corresponding lattice evolution are acquired by in/ex situ characterizations and measurements. These results contribute to nanowire mechanical design and also expand to strain-regulated three-dimensional multifunctional nanosystems.

15.
Small ; 18(50): e2204875, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36316239

ABSTRACT

The insertion type materials are the most important anode materials for lithium-ion batteries, but their insufficient capacity is the bottleneck of practical application. Here, LiAl5 O8 nanowires with high theoretical capacity and Li-ions diffusion coefficient are prepared and studied as an insertion anode material, which exhibits zero-strain properties upon electrochemical cycling. However, the poor electronic conductivity of LiAl5 O8 definitely sacrifices the capacity and limits the rate performance. Therefore, compact LiAl5 O8 and carbon composite are further synthesized, in which nanosized LiAl5 O8 particles are uniformly embedded in an amorphous carbon matrix. It displays a reversible capacity of 490.9 mAh g-1 at 1 A g-1 , and the capacity rises continuously to 996.8 mAh g-1 after 1000 cycles due to the interfacial storage mechanism, that the excess Li+ ions can be accommodated in the grain boundaries and C/LiAl5 O8 interfaces.

16.
Langmuir ; 37(28): 8426-8434, 2021 Jul 20.
Article in English | MEDLINE | ID: mdl-34233119

ABSTRACT

CuCo2O4, a type of promising lithium-ion storage material, exhibits high electrochemical properties in lithium-ion batteries and enormous economic benefits. However, its practical application is limited by problems such as structural collapse and electrochemical stability during the charging and discharging process. In this work, the reduced graphene oxide (rGO)-coated CuCo2O4 (CuCo2O4/rGO) hollow microspheres were successfully prepared by electrostatic self-assembly. The CuCo2O4/rGO electrode shows an outstanding capability for lithium-ion storage and a remarkable rate capacity, e.g., 445 mA h g-1 at 5 A g-1. After 150 cycles at 0.1 A g-1, the reversible capacity of the CuCo2O4/rGO electrode is as high as 1080 mA h g-1, and it can still retain about 530 mA h g-1 in the 400th cycle at 1 A g-1. The hollow microspheres with mesoporous shells can cause electrolyte penetration into the spherical shell to effectively shorten the transfer distance of lithium ions, and the encapsulation of graphene improves the conductivity and stability of CuCo2O4, which endows CuCo2O4/rGO with a wonderful Li+ storage performance. It is proved that this is an efficient method to improve the electrochemical performance of metal compounds for better applications in energy storage.

17.
J Org Chem ; 86(9): 6698-6710, 2021 05 07.
Article in English | MEDLINE | ID: mdl-33881860

ABSTRACT

A copper-catalyzed, ligand-free intramolecular C-N coupling of (E)-2-(2-bromophenyl)-3-arylacrylamides has been developed. This protocol provides an efficient and practical synthetic route for the biologically important (E)-3-arylideneindolin-2-ones from o-bromophenylacetic acids and aromatic or conjugated alkenyl aldehydes. Readily available starting materials, mild and noble metal-free conditions, high efficiency, and good tolerability for phenolic hydroxyl groups make this approach attractive and applicable.


Subject(s)
Aldehydes , Copper , Catalysis , Ligands
18.
Phys Chem Chem Phys ; 24(1): 180-190, 2021 Dec 22.
Article in English | MEDLINE | ID: mdl-34878473

ABSTRACT

Lithium-sulfur battery is one of the most promising applicants for the next generation of energy storage devices whose commercial applications are impeded by the key issue of the shuttle effect. To overcome this obstacle, various two-dimensional (2D) carbon-based metal-free compounds have been proposed to serve as anchoring materials for immobilizing soluble lithium polysulfides (LiPs), which however suffer from low electronic conductivity implying unsatisfactory performance for catalyzing sulfur redox. Therefore, we have predicted metallic C5N monolayers, possessing hexagonal (H) and orthorhombic (O) phases, exhibiting excellent performance for suppressing the shuttle effect. First-principles simulations demonstrate that O-C5N could serve as a bifunctional anchoring material due to its strong adsorption capability to LiPs and excellent catalytic performance for sulfur redox with active sites from both basal plane and zigzag edges. Furthermore, the rate of Li2S oxidation over O-C5N is fast due to the low energy barrier of 0.93 eV for Li2S decomposition. While for H-C5N, only N atoms located at the armchair edges can efficiently trap LiPs and boost the formation and dissociation of Li2S during discharge and charge processes, respectively. The current work opens an avenue of designing 2D metallic carbon-based anchoring materials for lithium-sulfur batteries, which deserves further experimental research efforts.

19.
Environ Monit Assess ; 193(8): 512, 2021 Jul 24.
Article in English | MEDLINE | ID: mdl-34302554

ABSTRACT

Eight national air quality monitoring stations were selected to examine the environmental effects of prohibiting fireworks and firecrackers since January 1, 2018, in Jinan, China, by using an air quality index (AQI) on three time scales. In 2014-2018, the average annual AQI decreased year on year, but a downward trend in 2018 was only found by applying a Daniel trend test. The change in monthly data for 2016-2018 followed a "W" pattern. The overall AQI value was lower on New Year's Eve than during Spring Festival, and the 2-day AQI in 2018 was lower than that in 2017. The GIS analysis method was used for spatial visualization. The AQI in the built-up part of Jinan was high in the west and low in the east on New Year's Eve and Spring Festival of 2017, being lowest in the Development Zone. The AQI spatial distribution was high in the city core but low in its periphery; in 2018, the high-AQI center appeared near the Provincial Seed Warehouse on New Year's Eve and Spring Festival. Multiple linear regression was used to analyze the relationship between AQI and pollutants. Six pollutants were found to be positively correlated with the AQI. PM2.5 and PM10 had the strongest correlations on New Year's Eve and Spring Festival, for which the correlations of SO2, CO, and NO2 were significantly weaker in 2018 than in 2017.


Subject(s)
Air Pollutants , Air Pollution , Air Pollutants/analysis , Air Pollution/analysis , China , Cities , Environmental Monitoring , Particulate Matter/analysis
20.
Small ; 16(23): e1907556, 2020 Jun.
Article in English | MEDLINE | ID: mdl-32378323

ABSTRACT

Carbides are commonly regarded as efficient hydrogen evolution reaction (HER) catalysts, but their poor oxygen evolution reaction (OER) catalytic activities seriously limit their practical application in overall water splitting. Here, vertically aligned porous cobalt tungsten carbide nanosheet embedded in N-doped carbon matrix (Co6 W6 C@NC) is successfully constructed on flexible carbon cloth (CC) as an efficient bifunctional electrocatalyst for overall water splitting via a facile metal-organic framework (MOF) derived method. The synergistic effect of Co and W atoms effectively tailors the electron state of carbide, optimizing the hydrogen-binding energy. Thus Co6 W6 C@NC shows an enhanced HER performance with an overpotential of 59 mV at a current density of -10 mA cm-2 . Besides, Co6 W6 C@NC easily in situ transforms into tungsten actived cobalt oxide/hydroxide during the OER process, serving as OER active species, which provides an excellent OER activity with an overpotential of 286 mV at a current density of -10 mA cm-2 . The water splitting device, by applying Co6 W6 C@NC as both the cathode and anode, requires a low cell voltage of 1.585 V at 10 mA cm-2 with the great stability in alkaline solution. This work provides a feasible strategy to fabricate bimetallic carbides and explores their possibility as bifunctional catalysts toward overall water splitting.

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