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
.
We report phase-programmable Gaussian boson sampling (GBS) which produces up to 113 photon detection events out of a 144-mode photonic circuit. A new high-brightness and scalable quantum light source ...is developed, exploring the idea of stimulated emission of squeezed photons, which has simultaneously near-unity purity and efficiency. This GBS is programmable by tuning the phase of the input squeezed states. The obtained samples are efficiently validated by inferring from computationally friendly subsystems, which rules out hypotheses including distinguishable photons and thermal states. We show that our GBS experiment passes a nonclassicality test based on inequality constraints, and we reveal nontrivial genuine high-order correlations in the GBS samples, which are evidence of robustness against possible classical simulation schemes. This photonic quantum computer, Jiuzhang 2.0, yields a Hilbert space dimension up to ∼ 1043, and a sampling rate ∼ 1024 faster than using brute-force simulation on classical supercomputers.
Solid/liquid interfaces are ubiquitous in nature and knowledge of their atomic-level structure is essential in elucidating many phenomena in chemistry, physics, materials science and Earth science
. ...In electrochemistry, in particular, the detailed structure of interfacial water, such as the orientation and hydrogen-bonding network in electric double layers under bias potentials, has a significant impact on the electrochemical performances of electrode materials
. To elucidate the structures of electric double layers at electrochemical interfaces, we combine in situ Raman spectroscopy and ab initio molecular dynamics and distinguish two structural transitions of interfacial water at electrified Au single-crystal electrode surfaces. Towards negative potentials, the interfacial water molecules evolve from structurally 'parallel' to 'one-H-down' and then to 'two-H-down'. Concurrently, the number of hydrogen bonds in the interfacial water also undergoes two transitions. Our findings shed light on the fundamental understanding of electric double layers and electrochemical processes at the interfaces.
Aqueous rechargeable Zn metal batteries have attracted widespread attention due to the intrinsic high volumetric capacity, low cost, and high safety. However, the low Coulombic efficiency and limited ...lifespan of Zn metal anodes resulting from uncontrollable growth of Zn dendrites impede their practical application. In this work, a 3D interconnected ZnF2 matrix is designed on the surface of Zn foil (Zn@ZnF2) through a simple and fast anodic growth method, serving as a multifunctional protective layer. The as‐fabricated Zn@ZnF2 electrode can not only redistribute the Zn2+ ion flux, but also reduce the desolvation active energy significantly, leading to stable and facile Zn deposition kinetics. The results reveal that the Zn@ZnF2 electrode can effectively inhibit dendrites growth, restrain the hydrogen evolution reactions, and endow excellent plating/stripping reversibility. Accordingly, the Zn@ZnF2 electrode exhibits a long cycle life of over 800 h at 1 mA cm−2 with a capacity of 1.0 mAh cm−2 in a symmetrical cell test, the feasibility of which is also convincing in Zn@ZnF2//MnO2 and Zn@ZnF2//V2O5 full batteries. Importantly, a hybrid zinc‐ion capacitor of the Zn@ZnF2//AC can work at an ultrahigh current density of ≈60 mA cm−2 for up to 5000 cycles with a high capacity retention of 92.8%.
A 3D interconnected ZnF2 matrix on the surface of Zn foil (Zn@ZnF2) is prepared through a simple and fast electrochemical anodic growth method. The as‐fabricated Zn@ZnF2 electrode can not only redistribute the Zn2+ ion flux, but also reduce the desolvation active energy significantly, leading to stable and facile Zn deposition kinetics.
Rechargeable zinc‐ion batteries (ZIBs) are emerging as a promising alternative for Li‐ion batteries. However, the developed cathodes suffer from sluggish Zn2+ diffusion kinetics, leading to poor rate ...capability and inadequate cycle life. Herein, an in situ polyaniline (PANI) intercalation strategy is developed to facilitate the Zn2+ (de)intercalation kinetics in V2O5. In this way, a remarkably enlarged interlayer distance (13.90 Å) can be constructed alternatively between the VO layers, offering expediting channels for facile Zn2+ diffusion. Importantly, the electrostatic interactions between the Zn2+ and the host O2−, which is another key factor in hindering the Zn2+ diffusion kinetics, can be effectively blocked by the unique π‐conjugated structure of PANI. As a result, the PANI‐intercalated V2O5 exhibits a stable and highly reversible electrochemical reaction during repetitive Zn2+ insertion and extraction, as demonstrated by in situ synchrotron X‐ray diffraction and Raman studies. Further first‐principles calculations clearly reveal a remarkably lowered binding energy between Zn2+ and host O2−, which explains the favorable kinetics in PANI‐intercalated V2O5. Benefitting from the above, the overall electrochemical performance of PANI‐intercalated V2O5 electrode is remarkable improved, exhibiting excellent high rate capability of 197.1 mAh g−1 at current density of 20 A g−1 with capacity retention of 97.6% over 2000 cycles.
An in situ polyaniline (PANI) intercalation strategy is developed to facilitate the Zn2+ (de)intercalation kinetics in V2O5. PANI not only expands the diffusion channels for facilitating Zn2+ diffusion, but also maintains the structural stability as interlayer pillars. Especially, its unique π‐conjugated structure, serving as electron‐reservoir, simultaneously shields the electrostatic interactions between Zn2+ and V2O5 host.
Rechargeable aqueous metal-ion batteries are very promising as alternative energy storage devices during the post-lithium-ion era because of their green and safe inherent features. Among the ...different aqueous metal-ion batteries, aqueous zinc-ion batteries (ZIBs) have recently been studied extensively due to their unique and outstanding benefits that hold promise for large-scale power storage systems. However, zinc anode problems in ZIBs, such as zinc dendrites and side reactions, severely shorten the ZIB's cycle lifetime, thus restricting their practical application. Here, we sum up in detail the recent progress on general strategies to suppress zinc dendrites and zinc anode side reactions based on advanced materials and structure design, including the modification of the planar zinc electrode surface layer, internal structural optimization of the zinc bulk electrode, modification of the electrolyte and construction of the multifunctional separator. The various functional materials, structures and battery efficiencies are discussed. Finally, the challenges for ZIBs are identified in the production of functional zinc anodes.
This review summarizes recent progresses in material and structural designs of zinc anodes for high-performance aqueous zinc-ion batteries.
Currently, development of suitable cathode materials for zinc‐ion batteries (ZIBs) is plagued by the sluggish kinetics of Zn2+ with multivalent charge in the host structure. Herein, it is ...demonstrated that interlayer Mn2+‐doped layered vanadium oxide (Mn0.15V2O5·nH2O) composites with narrowed direct bandgap manifest greatly boosted electrochemical performance as zinc‐ion battery cathodes. Specifically, the Mn0.15V2O5·nH2O electrode shows a high specific capacity of 367 mAh g−1 at a current density of 0.1 A g−1 as well as excellent retentive capacities of 153 and 122 mAh g−1 after 8000 cycles at high current densities up to 10 and 20 A g−1, respectively. Even at a low temperature of −20 °C, a reversible specific capacity of 100 mAh g−1 can be achieved at a current density of 2.0 A g−1 after 3000 cycles. The superior electrochemical performance originates from the synergistic effects between the layered nanostructures and interlayer doping of Mn2+ ions and water molecules, which can enhance the electrons/ions transport kinetics and structural stability during cycling. With the aid of various ex situ characterization technologies and density functional theory calculations, the zinc‐ion storage mechanism can be revealed, which provides fundamental guidelines for developing high‐performance cathodes for ZIBs.
Vanadium oxide pillared by interlayer doping of Mn2+ ions and water is synthesized through a facile microwave‐assisted strategy. When evaluated as a cathode for zinc‐ion batteries, the as‐prepared electrode delivers superior zinc‐ion storage properties in terms of high specific capacity, stable cycling capability, excellent rate, and low‐temperature performance.
Rechargeable zinc‐ion batteries (ZIBs) have recently attracted attention for applications in energy storage systems owing to their intrinsic safety, low cost, environmental compatibility, and ...competitive gravimetric energy density. To enable the practical applications of ZIBs, their energy density must be equivalent to the existing commercial lithium‐ion batteries. To acquire high‐energy density, increasing the operating voltage of the battery is undoubtedly an effective method, which demands cathode material to exhibit a high voltage versus Zn2+/Zn, while matching a highly reversible anode and an electrolyte with a sufficiently wide electrochemical stability window. This review focuses on the design strategies and challenges towards high‐voltage ZIBs. First, the basic electrochemistry of ZIBs and the recent progress in various high‐voltage cathode materials for ZIBs, including Prussian blue analogs, polyanionic compounds, and metal‐based oxides are introduced. The challenges and corresponding countermeasures of these materials are discussed, while strategies to further improve the cathode operating voltage, influence factors of voltage in the redox reaction, and energy storage mechanism are also illustrated. The following section describes the strategies towards high‐performance Zn anode, and summarizes the electrolytes that can help increase the battery voltage. The final section outlines the potential development in ZIBs.
This review focuses on the recent advancements of high‐voltage zinc‐ion batteries in aspects of cathode materials, Zn anodes, and electrolytes. Special attention is given to the challenges, design strategies, voltage variation trend of Prussian blue analogs, polyanionic compounds, and metal‐based oxides. Electrolytes with a wide electrochemical stability window, relevant challenges, and strategies on highly reversible Zn anodes are also reviewed.
Immunosuppressive molecules are extremely valuable prognostic biomarkers across different cancer types. However, the diversity of different immunosuppressive molecules makes it very difficult to ...accurately predict clinical outcomes based only on a single immunosuppressive molecule. Here, we establish a comprehensive immune scoring system (ISS
) based on 6 immunosuppressive ligands (NECTIN2, CEACAM1, HMGB1, SIGLEC6, CD44, and CD155) using the LASSO method to improve prognostic accuracy and provide an additional selection strategy for adjuvant chemotherapy of gastric cancer (GC). The results show that ISS
is an independent prognostic factor and a supplement of TNM stage for GC patients, and it can improve their prognosis prediction accuracy; in addition, it can distinguish GC patients with better prognosis from those with high prognostic nutritional index score; furthermore, ISS
can also be used as a tool to select GC patients who would benefit from adjuvant chemotherapy independent of their TNM stages, MSI status and EBV status.
Despite the wide use of aryl radicals in organic synthesis, current methods to prepare them from aryl halides, carboxylic acids, boronic acids, and diazonium salts suffer from limitations. Aryl ...triflates, easily obtained from phenols, are promising aryl radical progenitors but remain elusive in this regard. Inspired by the single electron transfer process for aryl halides to access aryl radicals, we developed a simple and efficient protocol to convert aryl triflates to aryl radicals. Our success lies in exploiting sodium iodide as the soft electron donor assisted by light. This strategy enables the scalable synthesis of two types of important organic molecules, i.e., aryl boronates and aryl iodides, in good to high yields, with broad functional group compatibility in a transition-metal-free manner at room temperature. This protocol is anticipated to find potential applications in other aryl-radical-involved reactions by using aryl triflates as aryl radical precursors.
PDF
