Iron fluoride, an intercalation-conversion cathode for lithium ion batteries, promises a high theoretical energy density of 1922 Wh kg
However, poor electrochemical reversibility due to repeated ...breaking/reformation of metal fluoride bonds poses a grand challenge for its practical application. Here we report that both a high reversibility over 1000 cycles and a high capacity of 420 mAh g
can be realized by concerted doping of cobalt and oxygen into iron fluoride. In the doped nanorods, an energy density of ~1000 Wh kg
with a decay rate of 0.03% per cycle is achieved. The anion's and cation's co-substitutions thermodynamically reduce conversion reaction potential and shift the reaction from less-reversible intercalation-conversion reaction in iron fluoride to a highly reversible intercalation-extrusion reaction in doped material. The co-substitution strategy to tune the thermodynamic features of the reactions could be extended to other high energy conversion materials for improved performance.
LiNixCoyMnzO2 (x+y+z=1)||graphite lithium‐ion battery (LIB) chemistry promises practical applications. However, its low‐temperature (≤ −20 °C) performance is poor because the increased resistance ...encountered by Li+ transport in and across the bulk electrolytes and the electrolyte/electrode interphases induces capacity loss and battery failures. Though tremendous efforts have been made, there is still no effective way to reduce the charge transfer resistance (Rct) which dominates low‐temperature LIBs performance. Herein, we propose a strategy of using low‐polarity‐solvent electrolytes which have weak interactions between the solvents and the Li+ to reduce Rct, achieving facile Li+ transport at sub‐zero temperatures. The exemplary electrolyte enables LiNi0.8Mn0.1Co0.1O2||graphite cells to deliver a capacity of ≈113 mAh g−1 (98 % full‐cell capacity) at 25 °C and to remain 82 % of their room‐temperature capacity at −20 °C without lithium plating at 1/3C. They also retain 84 % of their capacity at −30 °C and 78 % of their capacity at −40 °C and show stable cycling at 50 °C.
Low‐polarity‐solvent electrolytes (LPSEs) 1) enable the formation of the anion‐derived interphases on both electrodes and 2) have weak interactions between the solvent molecules and Li+, which provide fast Li+ transport kinetics and reduced resistance in both charge transfer process and Li+ transport in electrode/electrolyte interphases, achieving excellent battery performance under both fast‐charge and low‐temperature conditions.
Since the inception of Bitcoin, cryptocurrencies and the underlying blockchain technology have attracted an increasing interest from both academia and industry. Among various core components, ...consensus protocol is the defining technology behind the security and performance of blockchain. From incremental modifications of Nakamoto consensus protocol to innovative alternative consensus mechanisms, many consensus protocols have been proposed to improve the performance of the blockchain network itself or to accommodate other specific application needs. In this survey, we present a comprehensive review and analysis on the state-of-the-art blockchain consensus protocols. To facilitate the discussion of our analysis, we first introduce the key definitions and relevant results in the classic theory of fault tolerance which help to lay the foundation for further discussion. We identify five core components of a blockchain consensus protocol, namely, block proposal, block validation, information propagation, block finalization, and incentive mechanism. A wide spectrum of blockchain consensus protocols are then carefully reviewed accompanied by algorithmic abstractions and vulnerability analyses. The surveyed consensus protocols are analyzed using the five-component framework and compared with respect to different performance metrics. These analyses and comparisons provide us new insights in the fundamental differences of various proposals in terms of their suitable application scenarios, key assumptions, expected fault tolerance, scalability, drawbacks and trade-offs. We believe this survey will provide blockchain developers and researchers a comprehensive view on the state-of-the-art consensus protocols and facilitate the process of designing future protocols.
Quantum computational advantage using photons Zhong, Han-Sen; Wang, Hui; Deng, Yu-Hao ...
Science (American Association for the Advancement of Science),
12/2020, Letnik:
370, Številka:
6523
Journal Article
Recenzirano
Odprti dostop
Quantum computers promise to perform certain tasks that are believed to be intractable to classical computers. Boson sampling is such a task and is considered a strong candidate to demonstrate the ...quantum computational advantage. We performed Gaussian boson sampling by sending 50 indistinguishable single-mode squeezed states into a 100-mode ultralow-loss interferometer with full connectivity and random matrix-the whole optical setup is phase-locked-and sampling the output using 100 high-efficiency single-photon detectors. The obtained samples were validated against plausible hypotheses exploiting thermal states, distinguishable photons, and uniform distribution. The photonic quantum computer,
, generates up to 76 output photon clicks, which yields an output state-space dimension of 10
and a sampling rate that is faster than using the state-of-the-art simulation strategy and supercomputers by a factor of ~10
.
Aqueous Zn batteries are promising energy storage devices for large-scale energy-storage due to low cost and high energy density. However, their lifespan is limited by the water decomposition and Zn ...dendrite growth. Here, we suppress water reduction and Zn dendrite growth in dilute aqueous electrolyte by adding dimethyl sulfoxide (DMSO) into ZnCl2–H2O, in which DMSO replaces the H2O in Zn2+ solvation sheath due to a higher Gutmann donor number (29.8) of DMSO than that (18) of H2O. The preferential solvation of DMSO with Zn2+ and strong H2O–DMSO interaction inhibit the decomposition of solvated H2O. In addition, the decomposition of solvated DMSO forms Zn12(SO4)3Cl3(OH)15·5H2O, ZnSO3, and ZnS enriched-solid electrolyte interphase (SEI) preventing Zn dendrite and further suppressing water decomposition. The ZnCl2–H2O–DMSO electrolyte enables Zn anodes in Zn||Ti half-cell to achieve a high average Coulombic efficiency of 99.5% for 400 cycles (400 h), and the Zn||MnO2 full cell with a low capacity ratio of Zn:MnO2 at 2:1 to deliver a high energy density of 212 Wh/kg (based on both cathode and anode) and maitain 95.3% of the capacity over 500 cycles at 8 C.
Aqueous Zn batteries promise high energy density but suffer from Zn dendritic growth and poor low‐temperature performance. Here, we overcome both challenges by using an eutectic 7.6 m ZnCl2 aqueous ...electrolyte with 0.05 m SnCl2 additive, which in situ forms a zincophilic/zincophobic Sn/Zn5(OH)8Cl2⋅H2O bilayer interphase and enables low temperature operation. Zincophilic Sn decreases Zn plating/stripping overpotential and promotes uniform Zn plating, while zincophobic Zn5(OH)8Cl2⋅H2O top‐layer suppresses Zn dendrite growth. The eutectic electrolyte has a high ionic conductivity of ≈0.8 mS cm−1 even at −70 °C due to the distortion of hydrogen bond network by solvated Zn2+ and Cl−. The eutectic electrolyte enables Zn∥Ti half‐cell a high Coulombic efficiency (CE) of >99.7 % for 200 cycles and Zn∥Zn cell steady charge/discharge for 500 h with a low overpotential of 8 mV at 3 mA cm−2. Practically, Zn∥VOPO4 batteries maintain >95 % capacity with a CE of >99.9 % for 200 cycles at −50 °C, and retain ≈30 % capacity at −70 °C of that at 20 °C.
A highly reversible Zn anode working at low temperature is achieved by introducing SnCl2 into eutectic ZnCl2 aqueous electrolyte to form a zincophilic–zincophobic interfacial layer on the Zn anode in situ. The bottom layer of Sn facilitates uniform Zn deposition, while the top layer of zincophobic Zn5(OH)8Cl2 H2O facilitates Zn2+ diffusion and avoids Zn dendrites. The eutectic composition enhances the low temperature conductivity.
In response to ecosystem degradation from rapid economic development, China began investing heavily in protecting and restoring natural capital starting in 2000. We report on China's first national ...ecosystem assessment (2000–2010), designed to quantify and help manage change in ecosystem services, including food production, carbon sequestration, soil retention, sandstorm prevention, water retention, flood mitigation, and provision of habitat for biodiversity. Overall, ecosystem services improved from 2000 to 2010, apart from habitat provision. China's national conservation policies contributed significantly to the increases in those ecosystem services.
Nickel‐rich layered materials LiNi1‐x‐yMnxCoyO2 are promising candidates for high‐energy‐density lithium‐ion battery cathodes. Unfortunately, they suffer from capacity fading upon cycling, especially ...with high‐voltage charging. It is critical to have a mechanistic understanding of such fade. Herein, synchrotron‐based techniques (including scattering, spectroscopy, and microcopy) and finite element analysis are utilized to understand the LiNi0.6Mn0.2Co0.2O2 material from structural, chemical, morphological, and mechanical points of view. The lattice structural changes are shown to be relatively reversible during cycling, even when 4.9 V charging is applied. However, local disorder and strain are induced by high‐voltage charging. Nano‐resolution 3D transmission X‐ray microscopy data analyzed by machine learning methodology reveal that high‐voltage charging induced significant oxidation state inhomogeneities in the cycled particles. Regions at the surface have a rock salt–type structure with lower oxidation state and build up the impedance, while regions with higher oxidization state are scattered in the bulk and are likely deactivated during cycling. In addition, the development of micro‐cracks is highly dependent on the pristine state morphology and cycling conditions. Hollow particles seem to be more robust against stress‐induced cracks than the solid ones, suggesting that morphology engineering can be effective in mitigating the crack problem in these materials.
Significant oxidation state inhomogeneities induced by high‐voltage charging are revealed for Ni‐rich Li ion battery cathode material by the machine‐learning methodology data analysis of nano‐resolution 3D transmission X‐ray microscopy. The formation and propagation of micro‐cracks are proven to be dependent on the morphology of secondary particles and cycling conditions.
In contrast to the wealth of asymmetric transformations for generating central chirality from alkyl radicals, the enantiocontrol over the allenyl radicals for forging axial chirality represents an ...uncharted domain. The challenge arises from the unique elongated linear configuration of the allenyl radicals that necessitates the stereo‐differentiation of remote motifs away from the radical reaction site. We herein describe a copper‐catalyzed asymmetric radical 1,4‐carboalkynylation of 1,3‐enynes via the coupling of allenyl radicals with terminal alkynes, providing diverse synthetically challenging tetrasubstituted chiral allenes. A chiral N,N,P‐ligand is crucial for both the reaction initiation and the enantiocontrol over the highly reactive allenyl radicals. The reaction features a broad substrate scope, covering a variety of (hetero)aryl and alkyl alkynes and 1,3‐enynes as well as radical precursors with excellent functional group tolerance.
A copper‐catalyzed asymmetric radical 1,4‐carboalkynylation of 1,3‐enynes is realized, providing diverse tetrasubstituted chiral allenes. The utilization of the copper/chiral N,N,P‐ligand is crucial for the enantiocontrol over the allenyl radicals, which is difficult due to their elongated linear configuration that necessitates the stereo‐differentiation of remote motifs away from the reaction site.
P2‐type layered oxides suffer from an ordered Na+/vacancy arrangement and P2→O2/OP4 phase transitions, leading them to exhibit multiple voltage plateaus upon Na+ extraction/insertion. The deficient ...sodium in the P2‐type cathode easily induces the bad structural stability at deep desodiation states and limited reversible capacity during Na+ de/insertion. These drawbacks cause poor rate capability and fast capacity decay in most P2‐type layered oxides. To address these challenges, a novel high sodium content (0.85) and plateau‐free P2‐type cathode‐Na0.85Li0.12Ni0.22Mn0.66O2 (P2‐NLNMO) was developed. The complete solid‐solution reaction over a wide voltage range ensures both fast Na+ mobility (10−11 to 10−10 cm2 s−1) and small volume variation (1.7 %). The high sodium content P2‐NLNMO exhibits a higher reversible capacity of 123.4 mA h g−1, superior rate capability of 79.3 mA h g−1 at 20 C, and 85.4 % capacity retention after 500 cycles at 5 C. The sufficient Na and complete solid‐solution reaction are critical to realizing high‐performance P2‐type cathodes for sodium‐ion batteries.
A high sodium content (0.85) and plateau‐free P2‐type cathode, Na0.85Li0.12Ni0.22Mn0.66O2, is developed for sodium‐ion batteries. The sodium content promises a large specific capacity of 123.4 mA h g−1 with an average working voltage as high as 3.5 V. The complete solid‐solution reaction over a wide voltage range ensures small volume variation (1.7 %) and fast Na+ kinetics (10−10 to 10−11 cm2 s−1), contributing to both excellent cycling stability and rate capability.
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