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1.
A challenge still remains to develop high‐performance and cost‐effective air electrode for Li‐O2 batteries with high capacity, enhanced rate capability and long cycle life (100 times or above) despite recent advances in this field. In this work, a new design of binder‐free air electrode composed of three‐dimensional (3D) graphene (G) and flower‐like δ‐MnO2 (3D‐G‐MnO2) has been proposed. In this design, graphene and δ‐MnO2 grow directly on the skeleton of Ni foam that inherits the interconnected 3D scaffold of Ni foam. Li‐O2 batteries with 3D‐G‐MnO2 electrode can yield a high discharge capacity of 3660 mAh g?1 at 0.083 mA cm?2. The battery can sustain 132 cycles at a capacity of 492 mAh g?1 (1000 mAh gcarbon ?1) with low overpotentials under a high current density of 0.333 mA cm?2. A high average energy density of 1350 Wh Kg?1 is maintained over 110 cycles at this high current density. The excellent catalytic activity of 3D‐G‐MnO2 makes it an attractive air electrode for high‐performance Li‐O2 batteries.  相似文献   

2.
While stretchable micro‐supercapacitors (MSCs) have been realized, they have suffered from limited areal electrochemical performance, thus greatly restricting their practical electronic application. Herein, a facile strategy of 3D printing and unidirectional freezing of a pseudoplastic nanocomposite gel composed of Ti3C2Tx MXene nanosheets, manganese dioxide nanowire, silver nanowires, and fullerene to construct intrinsically stretchable MSCs with thick and honeycomb‐like porous interdigitated electrodes is introduced. The unique architecture utilizes thick electrodes and a 3D porous conductive scaffold in conjunction with interacting material properties to achieve higher loading of active materials, larger interfacial area, and faster ion transport for significantly improved areal energy and power density. Moreover, the oriented cellular scaffold with fullerene‐induced slippage cell wall structure prompts the printed electrode to withstand large deformations without breaking or exhibiting obvious performance degradation. When imbued with a polymer gel electrolyte, the 3D‐printed MSC achieves an unprecedented areal capacitance of 216.2 mF cm?2 at a scan rate of 10 mV s?1, and remains stable when stretched up to 50% and after 1000 stretch/release cycles. This intrinsically stretchable MSC also exhibits high rate capability and outstanding areal energy density of 19.2 µWh cm?2 and power density of 58.3 mW cm?2, outperforming all reported stretchable MSCs.  相似文献   

3.
A hybrid nanoarchitecture aerogel composed of WS2 nanosheets and carbon nanotube‐reduced graphene oxide (CNT‐rGO) with ordered microchannel three‐dimensional (3D) scaffold structure was synthesized by a simple solvothermal method followed by freeze‐drying and post annealing process. The 3D ordered microchannel structures not only provide good electronic transportation routes, but also provide excellent ionic conductive channels, leading to an enhanced electrochemical performance as anode materials both for lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs). Significantly, WS2/CNT‐rGO aerogel nanostructure can deliver a specific capacity of 749 mA h g?1 at 100 mA g?1 and a high first‐cycle coulombic efficiency of 53.4% as the anode material of LIBs. In addition, it also can deliver a capacity of 311.4 mA h g?1 at 100 mA g?1, and retain a capacity of 252.9 mA h g?1 at 200 mA g?1 after 100 cycles as the anode electrode of SIBs. The excellent electrochemical performance is attributed to the synergistic effect between the WS2 nanosheets and CNT‐rGO scaffold network and rational design of 3D ordered structure. These results demonstrate the potential applications of ordered CNT‐rGO aerogel platform to support transition‐metal‐dichalcogenides (i.e., WS2) for energy storage devices and open up a route for material design for future generation energy storage devices.  相似文献   

4.
The search for earth‐abundant and high‐performance electrode materials for sodium‐ion batteries represents an important challenge to current battery research. 2D transition metal dichalcogenides, particularly MoS2, have attracted increasing attention recently, but few of them so far have been able to meet expectations. In this study, it is demonstrated that another phase of molybdenum sulfide—amorphous chain‐like MoS3—can be a better choice as the anode material of sodium‐ion batteries. Highly compact MoS3 particles infiltrated with carbon nanotubes are prepared via the facile acid precipitation method in ethylene glycol. Compared to crystalline MoS2, the resultant amorphous MoS3 not only exhibits impressive gravimetric performance—featuring excellent specific capacity (≈615 mA h g?1), rate capability (235 mA h g?1 at 20 A g?1), and cycling stability but also shows exceptional volumetric capacity of ≈1000 mA h cm?3 and an areal capacity of >6.0 mA h cm?2 at very high areal loadings of active materials (up to 12 mg cm?2). The experimental results are supported by density functional theory simulations showing that the 1D chains of MoS3 can facilitate the adsorption and diffusion of Na+ ions. At last, it is demonstrated that the MoS3 anode can be paired with an Na3V2(PO4)3 cathode to afford full cells with great capacity and cycling performance.  相似文献   

5.
Freestanding composite structures with embedded transition metal dichalcogenides (TMDCs) as the active material are highly attractive in the development of advanced electrodes for energy storage devices. Most 3D electrodes consist of a bilayer design involving a core–shell combination. To further enhance the gravimetric and areal capacities, a 3D trilayer design is proposed that has MoSe2 as the TMDC sandwiched in‐between an inner carbon nanotube (CNT) core and an outer carbon layer to form a CNT/MoSe2/C framework. The CNT core creates interconnected pathways for the e?/Na+ conduction, while the conductive inert carbon layer not only protects the corrosive environment between the electrolyte and MoSe2 but also is fully tunable for an optimized Na+ storage. This unique heterostructure is synthesized via a solvothermal‐carbonization approach. Due to annealing under a confined structural configuration, MoSe2 interlayer spaces are expanded to facilitate a faster Na+ diffusion. It is shown that an ≈3 nm thick carbon layer yielded an optimized anode for a sodium‐ion battery. The 3D porosity of the heterostructure remains intact after an intense densification process to produce a high areal capacity of 4.0 mAh cm?2 and a high mass loading of 13.9 mg cm?2 with a gravimetric capacity of 347 mAh g?1 at 500 mA g?1 after 500 cycles.  相似文献   

6.
Highly conductive and ultrathin 2D nanosheets are of importance for the development of portable electronics and electric vehicles. However, scalable production and rational design for highly electronic and ionic conductive 2D nanosheets still remain a challenge. Herein, an industrially adoptable fluid dynamic exfoliation process is reported to produce large quantities of ionic liquid (IL)‐functionalized metallic phase MoS2 (m‐MoS2) and defect‐free graphene (Gr) sheets. Hybrid 2D–2D layered films are also fabricated by incorporating Gr sheets into compact m‐MoS2 films. The incorporated IL functionalities and Gr sheets prevent aggregation and restacking of the m‐MoS2 sheets, thereby creating efficient and rapid ion and electron pathways in the hybrid films. The hybrid film with a high packing density of 2.02 g cm?3 has an outstanding volumetric capacitance of 1430.5 F cm?3 at 1 A g?1 and an extremely high rate capability of 80% retention at 1000 A g?1. The flexible supercapacitor assembled using a polymer‐gel electrolyte exhibits excellent resilience to harsh electrochemical and mechanical conditions while maintaining an impressive rate performance and long cycle life. Successful achievement of an ultrahigh volumetric energy density (1.14 W h cm?3) using an organic electrolyte with a wide cell voltage of ≈3.5 V is demonstrated.  相似文献   

7.
Owing to its high theoretical specific capacity (1166 mA h g?1) and particularly its advantage to be paired with a lithium‐metal‐free anode, lithium sulfide (Li2S) is regarded as a much safer cathode for next‐generation advanced lithium–sulfur (Li–S) batteries. However, the low conductivity of Li2S and particularly the severe “polysulfide shuttle” of lithium polysulfide (LiPS) dramatically hinder their practical application in Li–S batteries. To address such issues, herein a bifuctional 3D metal sulfide‐decorated carbon sponge (3DTSC), which is constructed by 1D carbon nanowires cross‐linked with 2D graphene nanosheets with high conductivity and polar 0D metal sulfide nanodots with efficient electrocatalytic activity and strong chemical adsorption capability for LiPSs, is presented. Benefiting from the well‐designed multiscale, multidimensional 3D porous nanoarchitecture with high conductivity, and efficient electrocatalytic and absorption ability, the 3DTSC significantly mitigates LiPS shuttle, improves the utilization of Li2S, and facilitates the transport of electrons and ions. As a result, even with a high Li2S loading of 8 mg cm?2, the freestanding 3DTSC‐Li2S cathode without a polymer binder and metallic current collector delivers outstanding electrochemical performance with a high areal capacity of 8.44 mA h cm?2.  相似文献   

8.
Selenium–sulfur solid solutions are a class of potential cathode materials for high energy batteries, since they have higher theoretical capacities than selenium and improved conductivity over sulfur. Here, a high‐performance cathode material by confining 70 wt% of SeS2 in a highly ordered mesoporous carbon (CMK‐3) framework with a polydopamine (PDA) protection sheath for novel Li–Se/S batteries is reported. With a relatively high SeS2 mass loading of 2.6–3 mg cm?2, the CMK‐3/SeS2@PDA cathode exhibits a high capacity of >1200 mA h g?1 at 0.2 A g?1, excellent C‐rate capability of 535 mA h g?1 at 5 A g?1, and prolonged life over 500 cycles. Benefitting from the unique advantages of SeS2 and the rationally designed host framework, this new cathode material demonstrates a feasible strategy to overcome the bottlenecks of current Li–S systems for high energy density rechargeable batteries.  相似文献   

9.
Traditional challenges of poor cycling stability and low Coulombic efficiency in Zinc (Zn) metal anodes have limited their practical application. To overcome these issues, this work introduces a single metal-atom design featuring atomically dispersed single copper (Cu) atoms on 3D nitrogen (N) and oxygen (O) co-doped porous carbon (CuNOC) as a highly reversible Zn host. The CuNOC structure provides highly active sites for initial Zn nucleation and further promotes uniform Zn deposition. The 3D porous architecture further mitigates the volume changes during the cycle with homogeneous Zn2+ flux. Consequently, CuNOC demonstrates exceptional reversibility in Zn plating/stripping processes over 1000 cycles at 2 and 5 mA cm−2 with a fixed capacity of 1 mAh cm−2, while achieving stable operation and low voltage hysteresis over 700 h at 5 mA cm−2 and 5 mAh cm−2. Furthermore, density functional theory calculations show that co-doping N and O on porous carbon with atomically dispersed single Cu atoms creates an efficient zincophilic site for stable Zn nucleation. A full cell with the CuNOC host anode and high loading V2O5 cathode exhibits outstanding rate-capability up to 5 A g−1 and a stable cycle life over 400 cycles at 0.5 A g−1.  相似文献   

10.
Growth, photosynthesis, dark respiration and pigment contents were monitored in adult sporophytes of the Antarctic brown alga Desmarestia menziesii J. Agardh grown under fluctuating Antarctic daylength conditions. Growth rates were closely coupled to daylength variations with values varying from 0.05% d?1 in winter condition (July-August) to 0.5% d?1 in early summer (December). Photosynthetic pigments had maximum values of 1.8 mg g?1 FW (chlorophyll a), 0.4 mg g?1 FW (chlorophyll c) and 0.9 mg g?1 FW (fucoxanthin) in summer. These changes were also closely related to individual size and biomass of the plants. Net photosynthesis (Pmax), on a fresh weight basis, showed a clear seasonal pattern with highest rates of 25μmol O2 g?1 FW h?1 in October and minima close to 9μmol O2 g?1 FW h?1 in April. Dark respiration was high in spring (13μmol O2 g?1 FW h?1) approximately coinciding with growth peaks. Likewise, photosynthetic efficiency (α) and the initial saturating light point of photosynthesis (lk) increased significantly in spring [1.3 μimol O2 g?1 FW h?1 (μmol m?2 s?1)?1 and 26μmol photons m?2 s?1, respectively]. In the case of α, no significant differences between fresh weight and Chl a based rates were found. The results of the present study are the first that demonstrate seasonality of physiological parameters in D. menziesii sporophytes and confirm also that phenology and physiology of macroalgae can be simulated in the laboratory. On the other hand this study adds new elements to the explanation of the life strategy of D. menziesii, in particular that algal growth and photosynthesis occur under a programmed seasonal pattern.  相似文献   

11.
Rechargeable aqueous zinc‐ion batteries (ZIBs) are appealing due to their high safety, zinc abundance, and low cost. However, developing suitable cathode materials remains a great challenge. Herein, a novel 2D heterostructure of ultrathin amorphous vanadium pentoxide uniformly grown on graphene (A‐V2O5/G) with a very short ion diffusion pathway, abundant active sites, high electrical conductivity, and exceptional structural stability, is demonstrated for highly reversible aqueous ZIBs (A‐V2O5/G‐ZIBs), coupling with unprecedented high capacity, rate capability, long‐term cyclability, and excellent safety. As a result, 2D A‐V2O5/G heterostructures for stacked ZIBs at 0.1 A g?1 display an ultrahigh capacity of 489 mAh g?1, outperforming all reported ZIBs, with an admirable rate capability of 123 mAh g?1 even at 70 A g?1. Furthermore, the new‐concept prototype planar miniaturized zinc‐ion microbatteries (A‐V2O5/G‐ZIMBs), demonstrate a high volumetric capacity of 20 mAh cm?3 at 1 mA cm?2, long cyclability; holding high capacity retention of 80% after 3500 cycles, and in‐series integration, demonstrative of great potential for highly‐safe microsized power sources. Therefore, the exploration of such 2D heterostructure materials with strong synergy is a reliable strategy for developing safe and high‐performance energy storage devices.  相似文献   

12.
An optimized scaffold based on silicon microtubes is designed to increase the surface capacity of 3D lithium‐ion microbatteries. High‐depth, mechanically robust microstructures are fabricated using microelectronic facilities. Conformal deposition of anatase TiO2 is achieved using atomic layer deposition, realizing the targeted improvement for microbatteries; a surface capacity of 0.2 mA h cm–2 at a charge rate of C/10 is obtained in standard liquid electrolyte. This work paves the way for the fabrication of solid‐state 3D Li‐ion microbatteries with an efficient 3D scaffold.  相似文献   

13.
Achieving a high areal capacity is essential for the transfer of outstanding laboratory electrode results to commercial applications and also to ensure there exists a capacity matched cathode and anode for a properly tuned battery. Despite intensive efforts, most electrode materials exhibit areal capacities lower than that of the graphite anodes (4 mA h cm?2). An effective and low‐cost approach is reported to attain a high areal capacity via an intense densification by compacting a porous carbon nanotube sponge grafted with Co3O4 nanoparticles. The hybrid sponge can be compacted to a large degree (up to a tenfold densification) while still keeping its structural integrity and the 3D porous network. This method allows achieving a mass loading of up ?to 14.3 mg cm?2 and an areal capacity of 12 mA h cm?2 (at a current density of 200 mA g?1) together with a gravimetric capacity of >800 mA h g?1. This densification by compaction approach offers an effective and low‐cost strategy to develop high mass loading and areal capacity electrodes for practical energy storage systems.  相似文献   

14.
Densely cross-linked poly(vinylamine) microbeads (∼2 μm) were prepared by precipitation copolymerization of N-vinyl formamide and ethylene glycoldimethacrylate in acetonitrile. The formamido groups of the microbeads were hydrolyzed into amino groups. Then, amino-functionalized microbeads were used for covalent immobilization of laccase via glutaraldehyde coupling. The average amount of immobilized enzyme was 18.7 mg/g microbeads. Kinetic parameters, Vmax and Km values were determined as 20.7 U/mg protein and 2.76 × 10−2 mmol/L for free enzyme and 15.8 U/mg protein and 4.65 mmol/L for the immobilized laccase, respectively. The immobilized laccase was operated in a batch reactor for the degradation of two different benzidine based dyes (i.e., Direct Blue 1 and Direct Red 128). The laccase immobilized on the microbeads was very effective for removal of these dyes which interfere with the hormonal system.  相似文献   

15.
Molybdenum disulfide (MoS2) has been recognized as a promising anode material for high‐energy Li‐ion (LIBs) and Na‐ion batteries (SIBs) due to its apparently high capacity and intriguing 2D‐layered structure. The low conductivity, unsatisfied mechanical stability, and limited active material utilization are three key challenges associated with MoS2 electrodes especially at high current rates and mass active material loading. Here, vertical MoS2 nanosheets are controllably patterned onto electrochemically exfoliated graphene (EG). Within the achieved hierarchical architecture, the intimate contact between EG and MoS2 nanosheets, interconnected network, and effective exposure of active materials by vertical channels simultaneously overcomes the above three problems, enabling high mechanical integrity and fast charge transport kinetics. Serving as anode material for LIBs, EG‐MoS2 with 95 wt% MoS2 content delivered an ultrahigh‐specific capacity of 1250 mA h g?1 after 150 stable cycles at 1 A g?1, which is among the highest values in all reported MoS2 electrodes, and excellent rate performance (970 mA h g?1 at 5 A g?1). Moreover, impressive cycling stability (509 mA h g?1 at 1 A g?1 after 250 cycles) and rate capability (423 mA h g?1 at 2 A g?1) were also achieved for SIBs. The area capacities reached 1.27 and 0.49 mA h cm?2 at ≈1 mA cm?2 for LIBs and SIBs, respectively. This work may inspire the development of new 2D hierarchical structures for high efficiency energy storage and conversion.  相似文献   

16.
Some elemental levels, morphological and photosynthetic characteristics and cellular metabolites of wheat plants (Triticum aestivum L. cv. Vergina) growing in the field on an ore body (Cu concentration in the soil 3050 ug g?1) were compared to control plants growing in the same environment where the Cu concentration in the soil was 140 μg g1. The concentrations of Cu, K, Pb, Zn, Mg and Fe were higher in the ore plants but Ca was lower. Growth of the ore plants was inhibited, with decreased height (25%), weight (5%), leaf area (7%) and leaf dry weight (5%) compared to the control plants. Leaf protein concentration of the ore plants was 16. 2 mg cm2 leaf area, 63% of that of the control plants. The ore plants were chlorotic and chlorophyll concentration was 3. 8 μg cm?2 leaf area, 6. 4 times lower than that in the control plants. Ribulose 1. 5-bisphosphate carboxylase/oxygenase (Rubisco, EC 4. 1. 1. 39) activity was 13. 4 μmol CO2 fixed (mg dry weight)?1 min?1, 164% of the activity in control plants. Therefore, growth inhibition did not appear to result from inhibition of the dark reactions of photosynthesis. High Rubisco activity appears to be maintained to permit maximal CO2 fixation rates whenever energy is available. Parameters of chlorophyll fluorescence Fm, Fv, I1/2 and Fv/Fm were lower in the ore-grown plants than in control plants; Fm was higher. These values indicate that there is a decrease in the pool size of the electron acceptors on the reducing side of photosystem II (PSII), a destruction of PSII centres and interference in the photochemistry of PSII. The nitrogen content, soluble sugars, starch and lipid content were lower in ore-grown plants. Lower carbohydrate levels appear to result from low photosynthetic activity. The fatty acid composition of lipids was similar in both groups. A lower proportion of polyunsaturated fatty acids was found in the ore-grown plants. Stress caused by high Cu concentration in the soil appears to affect the light reactions of photosynthesis leading to growth inhibition.  相似文献   

17.
A water soluble acidic heteropolysaccharide named WAF was isolated from Auricularia auricula‐judae by extracting with 0.9% NaCl solution. By using gas chromatography, gas chromatography‐mass spectrometry, and NMR, its chemical structure was determined to be composed of a backbone of α‐(1→3)‐linked D ‐mannopyranose residues with pendant side groups of β‐D ‐xylose, β‐D ‐glucose, or β‐D ‐glucuronic acid at position O6 or O2. Six fractions prepared from WAF with a weight‐average molecular mass (Mw) between 5.9 × 104 and 64.7 × 104 g/mol were characterized with laser light scattering and viscometry in 0.1M NaCl at 25°C. The dependence of intrinsic viscosity ([η]) and radius of gyration (Rg) on Mw for this polysaccharide were found to be [η] = 1.79 × 10?3Mw0.96 cm3 g?1 and Rg = 6.99 × 10?2 Mw0.54 nm. The molar mass per unit contour length (ML) and the persistence length (Lp) were estimated to be 1124 nm?1 and 11 nm, respectively. The WAF exhibited a semirigid character typical of linear polysaccharides. Molecular modeling was then used to predict the ordered and disordered states of WAF; the simulated ML and Lp were however much smaller than the experimental values. Taken altogether, the results suggested that WAF formed a duplex in solution. © 2010 Wiley Periodicals, Inc. Biopolymers 95: 217–227, 2011.  相似文献   

18.
Despite the 3–5 fold higher energy density than the conventional Li‐ion cells at a lower cost, commercialization of Li–S batteries is hindered by the insulating nature of sulfur and the dissolution of intermediate polysulfides (Li2S X , 4 < X ≤ 8) into the electrolyte. The authors demonstrate here multichannel carbon nanofibers that are composed of parallel mesoporous channels connected with micropores as sulfur containment. In addition, hydroxyl functional groups are formed on the carbon surface through a chemical activation to enhance the interaction between sulfur and carbon. In the sulfur embedded composite, the mesoporous multichannel enhances the active material utilization and sulfur loading, while the micropores act as a reaction chamber for sulfur component and trap site for polysulfide with the assistance of the functional groups. This sulfur–carbon composite electrode with 2.2 mg cm?2 sulfur displays excellent performance with high rate capability (initial capacity of 1351 mA h g?1 at C/5 rate and 847 mA h g?1 at 5C rate), maintaining 920 mA h g?1 even after 300 cycles (a decay of 0.07% per cycle). Furthermore, a stable reversible capacity of as high as ≈1100 mA h g?1 is realized with a higher sulfur loading of 4.6 mg cm?2.  相似文献   

19.
The volume expansion and dendrite growth of metallic Li anode during charge/discharge processes hinder its practical application in energy storage. Seeking an appropriate host for distributing bulk Li in a 3D manner is an effective way to solve these problems. Here, a novel porous graphene scaffold with cellular chambers for incorporating Li metal is presented. Using such a unique host, ultrathin Li layers of 3 µm in thickness are anchored on graphene to form porous microstructures, which provides much more reaction sites for Li ions compared with that of bulk Li, significantly promoting the reversibility of Li stripping and plating. Also the high current density can be effectively dissipated by the graphene scaffold to remarkably improve the rate capability of Li anode. The symmetrical Li cell using such a Li anode can run stably for 200 cycles at 5 mA cm?2 and even 70 cycles at 10 mA cm?2 in an unmodified carbonate‐based electrolyte, which has rarely been achieved in such aggressive working conditions. Lithium‐ion capacitor cells using this anode also show outstanding rate capability and cycling stability, which can work at an ultrahigh current density of 30 A g?1 and keep steady for over 4000 cycles at 3.75 A g?1.  相似文献   

20.
It has previously been found (1) that feeding rats a diet containing a high amount of sunflowerseed oil results in a higher coronary flow and left ventricular work of their isolated hearts as compared to hearts of rats fed hydrogenated coconut oil or lard. It was hypothesized that this phenomenon can be explained by an influence of dietary linoleic acid on prostaglandin synthesis in the heart. To verify this hypothesis rabbits and rats were fed for four weeks sunflowerseed oil (SSO), hydrogenated coconut oil (HCO) or lard (L) to a maximum of 30 to 40 per cent of the total digestable energy, and the prostaglandin release from the isolated perfused hearts and rat aortas was determined by gas chromatography and bio-assay (PGI2).For the isolated hearts of rabbits fed SSO, the release of PGE2, PGF and 6-oxo-PGF was 1.7, 0.7 and 3.0 ng min−1 g−1 dry weight respectively; when fed L, these values were 2.9, 1.1 and 5.6 ng min−1 g−1. For the isolated hearts of rats fed SSO, HCO or L, the total release of PGE2, PGD2, PGF and thromboxane B2 (TXB2) was 5.9, 5.8 and 5.6 ng min−1 g−1 respectively; the release of 6-oxo-PGF was 3.4, 5.7 and 6.4 ng min−1 g−1 respectively. Relatively, 26% PGE2, 13% PGD2, 8% PGF, 6% TXB2 and 47% 6-oxo-PGF were released. For the isolated aortas of rats fed SSO or HCO, the release of PGI2-like activity was 0.37 ± 0.05 and 0.49 ± 0.05 ng min−1 cm−2. The release of PGI2-like activity from hearts of EFA-deficient rats was about 20% of that from control hearts.We conclude that, although feeding sunflowerseed oil, with respect to feeding hydrogenated coconut oil or lard, does increase coronary flow and left ventricular work, it does not increase the basal prostaglandin production in the isolated rat or rabbit heart; instead there is a tendency for a lower PGI2 synthesis.  相似文献   

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