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1.
Access to uranium resources is critical to the sustainable development of nuclear energy. The ocean contains abundant uranium resources, but the marine biological pollution and the low concentration of uranium make it a giant challenge to extract uranium from seawater. On the foundation of selective uranium adsorption using high uranium-affinity groups, realizing the external-field improved uranium capture without extra energy consumption is highly attractive. A solar thermal collector with 3D ion-transport networks based on environmentally friendly biomass adsorption material is reported, which contains antibacterial adsorption ligands and photothermal graphene oxide. The antibacterial ability through an easy one-step reaction and the fast mass transfer caused by photothermal conversion collaboratively improve the original adsorption capacity of the hydrogel by 46.7%, reaching 9.18 mg g−1 after contact with natural seawater for 14 days. This study provides a universal strategy for the design of physical-fields-enhanced hydrogel adsorbents.  相似文献   

2.
Marine sponges are used as biomonitors of heavy metals contamination in coastal environment as they process large amounts of water and have a high capacity for accumulating heavy metals. Here, inspired by the unique physical and physiological features of marine sponges, a surface engineered synthetic sponge for the highly efficient harvesting of uranium from natural seawater is developed. An ultrathin poly(imide dioxime) (PIDO)/alginate (Alg) interpenetrating polymer network hydrogel layer is uniformly wrapped around the skeleton of a melamine sponge (MS) substrate through a simple dipping–drying–crosslinking process, providing the hybrid MS@PIDO/Alg sponge with excellent uranium adsorption performance and sufficient mechanical strength to withstand the harsh conditions of practical applications. The maximum adsorption capacity reaches 910.98 mg‐U g‐gel‐1 for the PIDO/Alg hydrogel layer and 291.51 mg‐U g‐sponge‐1 for the whole hybrid MS@PIDO/Alg sponge in uranium‐spiked natural seawater. The adsorption capacity measured after 56 d of exposure in 5 tons of natural seawater is evaluated to be 5.84 mg‐U g‐gel‐1 (1.87 mg‐U g‐sponge‐1). This novel approach shows great promise for the mass production of high‐performance sponge adsorbent for uranium recovery from natural seawater and nuclear waste.  相似文献   

3.
A porous organic framework containing well-defined donor–acceptor units, named donor–acceptor porous organic framework (D–A-POF), is successfully synthesized. The localized electric field gradient at the pore surface induced by the intramolecular donor–acceptor (D–A) interactions endows D–A-POF with excellent desulfurization capabilities. D–A-POF exhibits high adsorption capacity of 3-methylthiophene (12.26 mmol g−1, 392.32 mg S g−1) and 1-benzothiophene (793.65 mg g−1, 189.25 mg S g−1) with impressive adsorption selectivity. Density functional theory calculations provide compelling evidence of the preferential selective adsorption of aromatic thiophene sulfides in D–A-POF. In fixed-bed breakthrough experiments, D–A-POF demonstrates its ability to selectively capture thiophene sulfides from model gasoline, resulting in fuel with sulfide content below 10 ppb. The high stability and high desulfurization efficiency of D–A-POF make it promising as a new porous adsorbent for ultra-depth adsorption desulfurization.  相似文献   

4.
The earth-abundant hard carbons have drawn great concentration as potassium-ion batteries (KIBs) anode materials because of their richer K-storage sites and wider interlayer distance versus graphite, but suffer from a low electrochemical reversibility. Herein, the novel Se/N co-doped hard-carbon nanotubes (h-CNTs) with localized electron configuration are demonstrated by creating unique N Se C covalent bonds stemmed from the precise doping of Se atoms into carbon edges and the subsequent bonding with pyrrole-N. The strong electron-donating ability of Se atoms on d-orbital provides abundant free electrons to effectively relieve charge polarization of pyrrole-N-C bonds, which contributes to balance the K-ion adsorption/desorption, therefore greatly boosting reversible K-ion storage capacity. After filtering into self-standing anodes with weights of 1.5–12.4 mg cm−2, all of them deliver a high reversible gravimetric capacity of 341 ± 4 mAh g−1 at 0.2 A g−1 and a linear increasing areal capacity to 4.06 mAh cm−2. The self-standing anode can still maintain 209 mAh g−1 at 8.0 A g−1 (93.3% retention) for a long period of 2000 cycles with a constant Se/N content.  相似文献   

5.
Potassium-ion batteries (PIBs) are promising alternatives to lithium-ion batteries because of the advantage of abundant, low-cost potassium resources. However, PIBs are facing a pivotal challenge to develop suitable electrode materials for efficient insertion/extraction of large-radius potassium ions (K+). Here, a viable anode material composed of uniform, hollow porous bowl-like hard carbon dual doped with nitrogen (N) and phosphorus (P) (denoted as N/P-HPCB) is developed for high-performance PIBs. With prominent merits in structure, the as-fabricated N/P-HPCB electrode manifests extraordinary potassium storage performance in terms of high reversible capacity (458.3 mAh g−1 after 100 cycles at 0.1 A g−1), superior rate performance (213.6 mAh g−1 at 4 A g−1), and long-term cyclability (205.2 mAh g−1 after 1000 cycles at 2 A g−1). Density-functional theory calculations reveal the merits of N/P dual doping in favor of facilitating the adsorption/diffusion of K+ and enhancing the electronic conductivity, guaranteeing improved capacity, and rate capability. Moreover, in situ transmission electron microscopy in conjunction with ex situ microscopy and Raman spectroscopy confirms the exceptional cycling stability originating from the excellent phase reversibility and robust structure integrity of N/P-HPCB electrode during cycling. Overall, the findings shed light on the development of high-performance, durable carbon anodes for advanced PIBs.  相似文献   

6.
Metal–organic framework-derived metal phosphides with high capacity, facile synthesis, and morphology-controlled are considered as potential anodes for lithium/sodium-ion batteries. However, the severe volume expansion during cycling can cause the electrode material to collapse and reduce the cycle life. Here, novel CoP-C@MoS2/C nanocube composites are synthesized by vapor-phase phosphating and hydrothermal process. As the anode of LIBs, CoP-C@MoS2/C exhibits outstanding long-cycle performance of 369 mAh g−1 at 10 A g−1 after 2000 cycles. In SIBs, the composite also displays excellent rate capability of 234 mAh g−1 at 5 A g−1 and an ultra-high the capacity retention rate of 90.16% at 1 A g−1 after 1000 cycles. Through density functional theory, it is found that the S ions and P ions at the interface formed by CoP and MoS2 can serve as Na+/Li+ diffusion channels with an action of van der Waals force, have attractive characteristics such as high ion adsorption energy, low expansion rate and fast diffusion kinetics compared with MoS2. This study provides enlightenment for the reasonable design and development of lithium/sodium storage anode materials composited with MOF-derived metal phosphides and metal sulfides.  相似文献   

7.
Sunlight-driven photoreduction of the environmentally mobile uranyl (VI) to less soluble tetravalent uranium is of considerable value to environmental sustainability, yet the pursuit for high-performance semiconductors is plagued by the current disadvantages of inferior charge separation/migration. This study reports that a nickel single atom isolated on a sulfur-functionalized graphitic carbon nitride/reduced graphene oxide 2D heterostructure enables exceptional uranyl photoreduction. Under only 11 min of visible light irradiation, the single atom anchored semiconductor yields a high removal rate of 99.8% and a record-high extraction capacity of 4144 mg g−1 in uranyl-containing wastewater and seawater. Theoretical calculations confirm that the remarkable uranyl photoreduction originates from the synergetic effect of Ni single atoms and intimate heterojunction establishment that can not only promote the separation/migration of photoexcited carriers, but also greatly reduce the energy barrier of uranyl reduction. This study showcases the exciting potential of single atom semiconductors for efficient uranyl removal from uranium-contaminated aqueous environments.  相似文献   

8.
Sodium-metal batteries (SMBs) employing transition-metal-free cathodes are of great importance for energy storage applications that require low cost and high energy density. A strategy to enhance the energy density of transition-metal-free-cathode SMBs by transforming the electrolyte from a dead mass to an energy-storage contributor is reported. NaI is used for the partial substitution of NaClO4 in the electrolyte and thus provides the additional electrochemistry of I3/I redox couple to enhance battery performance. Graphene oxide (GO) encapsulated mesoporous (10 nm) carbon spheres (N-MCS@GO) that are nitrogen-doped (15.71 at%) are fabricated as the cathode for the I3/I redox enhanced SMBs. It is experimentally demonstrated that: the mesoporous structure increases the capacitive energy storage by providing a substantial interface that enhances the electrochemistry of I3/I redox couples; and encapsulation of the mesoporous carbon spheres with GO suppresses self-discharge and increases Coulombic efficiencies from 70.4% to 91.9%. In full-cell configuration, N-MCS@GO working with the NaI-activated electrolyte can deliver a capacity of 279.6 mAh g−1 with an energy density of 459.2 Wh kg−1 in 0.5–3 V at 200 mA g−1. I3/I redox in the full cell maintains its activity without obvious decay after 1000 cycles at 1 A g−1, highlighting the practical application of the I3/I redox enhanced SMBs.  相似文献   

9.
The inferior shuttle effect of intermediate lithium polysulfides and the sluggish kinetics of sulfur redox reaction are two serious puzzles for the application of lithium–sulfur batteries. Herein, energy band alignment is combined with oxygen vacancies engineering to obtain TiO2 anatase/rutile homojunction (A/R-TiO2) with effective immobilization and high-efficiency catalytic conversion of polysulfides. Theoretical calculations and experiments reveal that the near perfect energy band alignment in A/R-TiO2 is conducive to fluent charge transfer and high catalytic activity, while the rich oxygen vacancies are engineered to provide abundant active sites for anchoring and accelerating conversion of soluble polysulfides. As a result, a battery with A/R-TiO2-modified separator delivers a marked sulfur utilization (1210 mAh g−1 at 0.1 C and 689 mAh g−1 at 1 C, 3.75 mg cm−2) and a high capacity retention of 63% over 300 cycles at 0.5 C (3.25 mg cm−2). More importantly, the A/R-TiO2-modified separator endows the pouch cell with a high capacity of 128.5 mAh at 0.05 C with a lean electrolyte/sulfur ratio for practical application (S loading: 4 mg cm−2).  相似文献   

10.
Emerging adsorption technology shows great potential for Pb2+ removal in the human body because of its high adsorption efficiency and easy operation. However, biosafety concerns in the human body limit the development of adsorbents in integrated lead removal for acute poisoning in humans from the gastrointestinal tract and even the blood. In this work, highly bio-safe and natural saccharomyces cerevisiae cells are immobilized on the interworking natural regenerated cellulose nanofibers network for integrated lead removal in the human body. High intrinsic biosafety of the aerogel is guaranteed due to the biocompatibility of aerogel composition and the absence of cross-linking substances. Attributing to the porous structure of cellulose nanofibrous scaffolds, saccharomyces cerevisiae cells are protected from shedding, and considerable loading sites for saccharomyces cerevisiae cells are ensured. Simultaneously, abundant functional groups on the saccharomyces cerevisiae cells exhibit superior adsorption ability with a saturated adsorption capacity of lead ions as high as 107 mg g−1 in the aquatic environment. After adsorption, Pb2+ concentration decreases from 879.70 to 248.53 µg L−1 in the intestinal phase and from 400 to 186.29 µg L−1 (within a safe level) in blood, providing an attractive strategy for detoxification of integrated lead in the human body.  相似文献   

11.
A series of BiOClxIy solid solutions with bifunctional properties was prepared by a hydrolysis method. When used as potential adsorbents for removal of dyes in wastewater, the as prepared samples exhibited the excellent adsorption and photocatalytic abilities, which indicated that the removal ability had been restored completely without centrifugal separating or other chemical desorption methods. Especially to the sample 301 prepared with a 3:1 M ratio of Cl to I, its adsorption capacity could reach nearly 5.0 mg g−1 within 5 min, which was at least 3 times larger than that of the individual BiOX (ca. 1.3 mg g−1), and its degradation efficiency of high concentration (20 mg L−1) methyl orange (MO) was up to 100% after 50 min of visible light irradiation. The relevant characterization results revealed that not only high specific surface area but also the electron structure of interlayer could be the key factors for the high adsorption ability. The possible mechanism was also discussed.  相似文献   

12.
The superstructure composed of various functional building units is promising nanostructure for lithium-ion batteries (LIBs) anodes with extreme volume change and structure instability, such as silicon-based materials. Here, a top-down route to fabricate Si/SiO2@graphene superstructure is demonstrated through reducing silicalite-1 with magnesium reduction and depositing carbon layers. The successful formation of superstructure lies on the strong 3D network formed by the bridged-SiO2 matrix coated around silicon nanoparticles. Furthermore, the mesoporous Si/SiO2 with amorphous bridged SiO2 facilitates the deposition of graphene layers, resulting in excellent structural stability and high ion/electron transport rate. The optimized Si/SiO2@graphene superstructure anode delivers an outstanding cycling life for ≈1180 mAh g−1 at 2 A g−1 over 500 cycles, excellent rate capability for ≈908 mAh g−1 at 12 A g−1, great areal capacity for ≈7 mAh cm−2 at 0.5 mA cm−2, and extraordinary mechanical stability. A full cell test using LiFePO4 as the cathode manifests a high capacity of 134 mAh g−1 after 290 loops. More notably, a series of technologies disclose that the Si/SiO2@graphene superstructure electrode can effectively maintain the film between electrode and electrolyte in LIBs. This design of Si/SiO2@graphene superstructure elucidates a promising potential for commercial application in high-performance LIBs.  相似文献   

13.
Herein, a simple but effective self-growth strategy to simultaneously modulate the interlayer distance and lyophilicity of graphene layers, which results in ultrahigh potassium-storage performances for carbon materials, is reported. This strategy involves the uniform adsorption of individual metal ions on the oxygen-containing groups on graphene oxide via electrostatic/coordination interactions and in situ self-conversion reaction between the metal ions and the oxygen-containing groups to form lyophilic ultrasmall metal oxide nanoparticles modified/intercalated graphene skeleton (OM-G) with precisely regulated interlayer distance. The synergistic effect of expanded interlayer distance and enhanced lyophilicity is revealed for the first time to significantly reduce the ion diffusion barrier and enhance ion transport kinetics by experimental and theoretical analysis. As a result, such unique OM-G monolith as free-standing anode for potassium-ion battery (PIB) delivered an ultrahigh reversible capability of 496.4 mAh g−1 at 0.1 A g−1, excellent rate capability (306.6 mAh g−1 at 10 A g−1), and remarkable long-term cycling stability (96.3% capacity retention over 2000 cycles at 1 A g−1), which are not only much better than those of previous graphene/carbon materials but also among the best performances for all PIB anodes ever reported. This study provides new fundamental insights for boosting the electrochemical properties of electrode materials.  相似文献   

14.
The severe shuttle effect and the sluggish redox reaction kinetics are the two most urgent issues with lithium-sulfur batteries (LSBs). In this work, Se vacancy-rich molybdenum selenide-modified graphene aerogels are designed to serve as both cathode host (MoSe2-x@GA/S) and freestanding interlayers (MoSe2-x@GA) for LSBs. The graphene network-supported binder-free sulfur host maximizes electron conductivity/Li+ migration rate and alleviates bulk expansion. The defect-rich MoSe2-x with sulfiphilic-lithiophilic properties accelerates the nucleation and dissociation of Li2S, while the insertion of a bifunctional interlayer not only facilitates the adsorption and conversion of polysulfides but also regulates the uniform lithium deposition and inhibit the growth of lithium dendrites. As a result, the assembled MoSe2-x@GA/S+interlayer electrode obtains good feedback in terms of capacity enhancement and cycling stability, possessing a high initial discharge capacity of 1256.9 mA h g−1 at 0.2 C and a slow decay ratio of 0.024% per cycle at a high current density of 1 C after 1000 long-term cycling, and achieve high specific capacity (720.6 mA h g−1) at high sulfur loading (4.8 mg cm−2) and lean electrolyte (5.5 µL mg−1) conditions. This insightful work contributes new ideas for the design of binder-free sulfur host and the application of defective electrocatalytic engineering.  相似文献   

15.
Heteroatoms in the carbon matrix are generally considered as active sites to enhance potassium storage capacity, while their adverse effects on ion batteries remain unclear. Herein, a series of sulfur doped carbon (SCDPx) with adjustable S content and crystallinity are accurately synthesized in the closed autoclave by controlling the ratios of precursors. Electrochemical measurements exhibit that heteroatom sulfur displays double-edged electrochemical activities with a high initial potassium storage capacity but poor cycling stability for carbon anode. Combined with solid-state nuclear magnetic resonance (NMR), catalytic tests, and various ex-situ characterizations, it is demonstrated that abundant S in the carbon would not only form C S C bonds, acting as active sites to reversibly adsorb/desorb potassium ions for high capacity, but also significantly catalyze the reduction and decomposition of the electrolyte including KPF6 and ethylene carbonate/diethyl carbonate (EC/DEC) to form thicker solid electrolyte interface (SEI) and degrade electrolyte, resulting in rapid capacity decay. As a result, the optimized sample (SCDP2) with the appropriate sulfur doping content exhibits the best electrochemical performance with high capacity (688.4 mA h g−1 at 100 mA g−1), long-term cycling stability (198.4 mA h g−1 at 2000 mA g−1 after 10 000 cycles), and excellent rate capability (238.8 mA h g−1 at 5000 mA g−1).  相似文献   

16.
Organic electrode materials have attracted tremendous attention for potassium-ion batteries (PIBs). Whereas, high-performance anodes are scarcely reported. Herein, a novel hexaazatriphenylene potassium carboxylate (HAT-COOK) is proposed as anode materials for PIBs. The rich CN/CO bonds guarantee the high theoretical capacity. It is also demonstrated HAT-COOK is more compatible with the water-soluble binders than the hydrophobic fluoride binders, forming homogenous electrode film, maintaining structural integrity, and achieving stable cycling and excellent rate performance. With the compatible binder, each HAT-COOK molecule can involve 6-electron transfer, yielding a high reversible discharge capacity of 288 mAh g−1 at 50 mA g−1, excellent rate performance (105 mAh g−1 at 5000 mA g−1), and good cycling stability (143 mAh g−1 after 500 cycles at 500 mA g−1). These results highlight the importance of the delicate molecular design of organic molecules as well as the optimization of binders to achieve high-performance PIBs.  相似文献   

17.
Simultaneously attaining high gravimetric energy density (Eg) and volumetric energy density (Ev) in lithium-sulfur (Li–S) batteries is a longstanding challenge that has to be solved for practical application, which demands breakthroughs in electrode materials with optimized functionality and structure. Herein, anthraquinone-containing, reactive-type polymer tubes (PQT) that can be used to regulate the redox chemistry of sulfur species are designed and prepared for practical Li–S batteries. PQT favors a similar redox potential window as sulfur, which effectively facilitates the immobilization and conversion of sulfur species through a reversible lithiation/delithiation process. Its tubular structure and high tap density is vital to the fabrication of intact electrode with high sulfur loading and minimizing electrolyte intake during battery operation. With all these contributions, Li–S battery with PQT/S cathode exhibits a stable cycling capacity (73% at 2.0 C over 1000 cycles), remarkable rate performance (514.2 mAh g−1 at 10 C), and a high areal capacity of 7.20 mAh g−1 with high sulfur loading under lean electrolyte condition. More importantly, the assembled Li–S pouch cell delivers an Eg of 329 Wh kg−1 and an Ev of 401 Wh L−1, which meets the requirement for practical operation.  相似文献   

18.
The 3D covalent organic frameworks (COFs) have attracted considerable attention owing to their unique structural characteristics. However, most of 3D COFs have interpenetration phenomena, which will result in decreased surface area and porosities, and thus limited their applications in molecular/gas capture. Developing 3D COFs with non-fold interpenetration is challenging but significant because of the existence of non-covalent interactions between the adjacent nets. Herein, a new 3D COF (BMTA-TFPM-COF) with dia topology and non-fold interpenetration for Au ion capture is first demonstrated. The constructed COF exhibits a high Brunauer–Emmett–Teller surface area of 1924 m2 g−1, with the pore volume of 1.85 cm3 g−1. The high surface area and abundant cavities as well as the abundant exposed CN linkages due to the non-interpenetration enable to absorb Au3+ with high capacity (570.18 mg g−1), selectivity (99.5%), and efficiency (68.3% adsorption of maximum capacity in 5 min). This work provides a new strategy to design 3D COFs for ion capture.  相似文献   

19.
Adsorption-photocatalysis technology based on covalent organic frameworks (COFs) offers an alternative method for advancing the field of uranium extraction from seawater. When determining the photocatalytic activity of COFs, the binding energy of excitons (Eb) functions is the decisive factor. Nevertheless, the majority of reported COFs have a large Eb, which seriously restricts their application in the field of photocatalysis. Using a practical π-skeleton engineering strategy, the current study synthesizes three donor-acceptor olefin-linked COFs containing amidoxime units in an effort to minimize Eb. Theoretical and experimental results reveal that the construction of planar and continuous π-electron delocalization channels can significantly reduce Eb and promote the separation of electron-hole pairs, thereby enhancing the photocatalytic activities. Moreover, the Eb of the TTh-COF-AO with a planar π-skeleton donor is significantly reduced, and exhibits a substantially smaller Eb (38.4 meV). Under visible light irradiation, a high photo-enhanced uranium extraction capacity of 10.24 mg g−1 is achieved from natural seawater without the addition of sacrificial reagents, which is superior to the majority of olefin-linked COFs that have been reported to date. This study, therefore, paves the way for the development of tailored, efficient COFs photocatalysts for the extraction of uranium from seawater.  相似文献   

20.
Silicon monoxide (SiO) is attaining extensive interest amongst silicon-based materials due to its high capacity and long cycle life; however, its low intrinsic electrical conductivity and poor coulombic efficiency strictly limit its commercial applications. Here low-cost coal-derived humic acid is used as a feedstock to synthesize in situ graphene-coated disproportionated SiO (D-SiO@G) anode with a facile method. HR-TEM and XRD confirm the well-coated graphene layers on a SiO surface. Scanning transmission X-ray microscopy and X-ray absorption near-edge structure spectra analysis indicate that the graphene coating effectively hinders the side-reactions between the electrolyte and SiO particles. As a result, the D-SiO@G anode presents an initial discharge capacity of 1937.6 mAh g−1 at 0.1 A g−1 and an initial coulombic efficiency of 78.2%. High reversible capacity (1023 mAh g−1 at 2.0 A g−1), excellent cycling performance (72.4% capacity retention after 500 cycles at 2.0 A g−1), and rate capability (774 mAh g−1 at 5 A g−1) results are substantial. Full coin cells assembled with LiFePO4 electrodes and D-SiO@G electrodes display impressive rate performance. These results indicate promising potential for practical use in high-performance lithium-ion batteries.  相似文献   

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