Due to its significant applications in many relevant fields, light detection in the solar‐blind deep‐ultraviolet (DUV) wavelength region is a subject of great interest for both scientific and ...industrial communities. The rapid advances in preparing high‐quality ultrawide‐bandgap (UWBG) semiconductors have enabled the realization of various high‐performance DUV photodetectors (DUVPDs) with different geometries, which provide an avenue for circumventing numerous disadvantages in traditional DUV detectors. This article presents a comprehensive review of the applications of inorganic UWBG semiconductors for solar‐blind DUV light detection in the past several decades. Different kinds of DUVPDs, which are based on varied UWBG semiconductors including Ga2O3, MgxZn1−xO, III‐nitride compounds (AlxGa1−xN/AlN and BN), diamond, etc., and operate on different working principles, are introduced and discussed systematically. Some emerging techniques to optimize device performance are addressed as well. Finally, the existing techniques are summarized and future challenges are proposed in order to shed light on development in this critical research field.
Recent advances in developing solar‐blind deep ultraviolet light (DUV) photodetectors based on various inorganic ultrawide‐bandgap semiconductors are reviewed, such as Ga2O3, MgxZn1−xO, III‐nitride compounds (AlxGa1−xN/AlN and BN), and diamonds.
Chiral tertiary alcohols are an important class of organic compounds which have found wide applications in both academia and industry. Therefore, various synthetic strategies towards these compounds ...have already been developed. Among them, the catalytic asymmetric addition of carbon nucleophiles to ketones is the most desirable route owing to its straightforwardness as well as its economic, efficient and versatile advantages. This review summarizes and discusses the recent achievements in this field classified according to the reaction types. Special attention is paid to the mechanisms, advantages and limitations of each reaction. In addition, the applications of these catalytic processes in the synthesis of related natural products, pharmaceuticals or their analogues are briefly discussed as well.
Covalent organic frameworks (COF) possess a robust and porous crystalline structure, making them an appealing candidate for energy storage. Herein, we report an exfoliated polyimide COF composite ...(P‐COF@SWCNT) prepared by an in situ condensation of anhydride and amine on the single‐walled carbon nanotubes as advanced anode for potassium‐ion batteries (PIBs). Numerous active sites exposed on the exfoliated frameworks and the various open pathways promote the highly efficient ion diffusion in the P‐COF@SWCNT while preventing irreversible dissolution in the electrolyte. During the charging/discharging process, K+ is engaged in the carbonyls of imide group and naphthalene rings through the enolization and π‐K+ effect, which is demonstrated by the DFT calculation and XPS, ex‐situ FTIR, Raman. As a result, the prepared P‐COF@SWCNT anode enables an incredibly high reversible specific capacity of 438 mA h g−1 at 0.05 A g−1 and extended stability. The structural advantage of P‐COF@SWCNT enables more insights into the design and versatility of COF as an electrode.
We prepare a polyimide covalent organic framework composite anode by effective in‐situ condensation of anhydride and amine on the surface of single‐walled carbon nanotubes. The construction of the conductive network accelerates the transport of electron. Dual electroactive sites in the framework, carbonyls and aromatic naphthalene rings, could store more potassium ions by the enolization and π‐K+ effect.
Herein, we highlight redox‐inert Zn2+ in spinel‐type oxide (ZnXNi1−XCo2O4) to synergistically optimize physical pore structure and increase the formation of active species on the catalyst surface. ...The presence of Zn2+ segregation has been identified experimentally and theoretically under oxygen‐evolving condition, the newly formed VZn−O−Co allows more suitable binding interaction between the active center Co and the oxygenated species, resulting in superior ORR performance. Moreover, a liquid flow Zn–air battery is constituted employing the structurally optimized Zn0.4Ni0.6Co2O4 nanoparticles supported on N‐doped carbon nanotube (ZNCO/NCNTs) as an efficient air cathode, which presents remarkable power density (109.1 mW cm−2), high open circuit potential (1.48 V vs. Zn), excellent durability, and high‐rate performance. This finding could elucidate the experimentally observed enhancement in the ORR activity of ZnXNi1−XCo2O4 oxides after the OER test.
The outstanding electrocatalytic performance of Zn0.4Ni0.6Co2O4/NCNTs towards ORR/OER is validated, presenting remarkable rate capability and durability in liquid‐flow Zn–air batteries. A dual‐reinforcement mechanism in the Zn–Ni–Co ternary spinel is also proposed. Zn0.4Ni0.6Co2O4/NCNTs exhibits extreme durability and electrochemically enhanced properties, enabling its application in practical rechargeable zinc–air batteries.
Transition‐metal oxides as electrocatalysts for the oxygen evolution reaction (OER) provide a promising route to face the energy and environmental crisis issues. Although palmeirite oxide A2Mo3O8 as ...OER catalyst has been explored, the correlation between its active sites (tetrahedral or octahedral) and OER performance has been elusive. Now, magnetic Co2Mo3O8@NC‐800 composed of highly crystallized Co2Mo3O8 nanosheets and ultrathin N‐rich carbon layer is shown to be an efficient OER catalyst. The catalyst exhibits favorable performance with an overpotential of 331 mV@10 mA cm−2 and 422 mV@40 mA cm−2, and a full water‐splitting electrolyzer with it as anode catalyst shows a cell voltage of 1.67 V@10 mA cm−2 in alkaline. Combined HAADFSTEM, magnetic, and computational results show that factors influencing the OER performance can be attributed to the tetrahedral Co sites (high spin, t23e4), which improve the OER kinetics of rate‐determining step to form *OOH.
Magnetic Co2Mo3O8@NC‐800 composed of single‐crystal Co2Mo3O8 and ultrathin nitrogen‐rich carbon was synthesized to uncover its OER active sites (Td Co2+ or Oh Co2+). Electrochemical data, magnetism data, and computations suggest that the Td Co2+ atoms (high spin, t23e4) in Co2Mo3O8 act as active sites facilitating the rate‐determining step, forming *OOH to promote the reaction kinetics for OER.
Bimetallic cobalt‐based spinel is sparking much interest, most notably for its excellent bifunctional performance. However, the effect of Fe3+ doping in Co3O4 spinel remains poorly understood, mainly ...because the surface state of a catalyst is difficult to characterize. Herein, a bifunctional oxygen electrode composed of spinel Co2FeO4/(Co0.72Fe0.28)Td(Co1.28Fe0.72)OctO4 nanoparticles grown on N‐doped carbon nanotubes (NCNTs) is designed, which exhibits superior performance to state‐of‐the‐art noble metal catalysts. Theoretical calculations and magnetic measurements reveal that the introduction of Fe3+ ions into the Co3O4 network causes delocalization of the Co 3d electrons and spin‐state transition. Fe3+ ions can effectively activate adjacent Co3+ ions under the action of both spin and charge effect, resulting in the enhanced intrinsic oxygen catalytic activity of the hybrid spinel Co2FeO4. This work provides not only a promising bifunctional electrode for zinc–air batteries, but also offers a new insight to understand the Co‐Fe spinel oxides for oxygen electrocatalysis.
A bifunctional oxygen electrode composed of hybrid spinel Co2FeO4 nanoparticles grown on N‐doped carbon nanotubes is a promising candidate for zinc–air batteries. Theoretical calculations and magnetic measurements reveal that the introduction of Fe cations into the Co3O4 network causes Co 3d electron delocalization and spin‐state transition, resulting in enhanced catalytic activity of the as‐prepared spinel Co2FeO4.
Conventional ion batteries utilizing metallic ions as the single charge carriers are limited by the insufficient abundance of metal resources. Although supercapacitors apply both cations and anions ...to store energy through absorption and/or Faradic reactions occurring at the interfaces of the electrode/electrolyte, the inherent low energy density hinders its application. The graphite‐cathode‐based dual‐ion battery possesses a higher energy density due to its high working potential of nearly 5 V. However, such a battery configuration suffers from severe electrolyte decomposition and exfoliation of the graphite cathode, rendering an inferior cycle life. Herein, a new surface‐modification strategy is developed to protect the graphite cathode from the anion salvation effect and the deposition derived from electrolyte decomposition by generating an artificial solid electrolyte interphase (SEI). Such SEI‐modified graphite exhibits superior cycling stability with 96% capacity retention after 500 cycles under 200 mA g−1 at the upper cutoff voltage of 5.0 V, which is much improved compared with the pristine graphite electrode. Through several ex situ studies, it is revealed that the artificial SEI greatly stabilizes the interfaces of the electrode/electrolyte after reconstruction and gradual establishment of the optimal anion‐transport path. The findings shed light on a new avenue toward promoting the performance of the dual‐ion battery (DIB) and hence to make it practical finally.
An artificial layer of a solid electrolyte interphase is fabricated on a graphite cathode for a dual‐ion battery (DIB). Such surface modification can alleviate the electrolyte decomposition at the high working voltage of the anion de‐/intercalation processes and the solvation effect of anions, much improving the cycling stability of the Li//graphite DIB.
Background
The prognosis of patients who have Epstein‐Barr virus (EBV)‐related nasopharyngeal carcinoma (NPC) in which the tumor tissues harbor EBV have a better prognosis than those without ...EBV‐related NPC. Therefore, the eighth edition of the TNM staging system could be modified for EBV‐related NPC by incorporating the measurement of plasma EBV DNA.
Methods
In total, 979 patients with NPC who received intensity‐modulated radiotherapy (IMRT) were retrospectively reviewed. Recursive partitioning analysis was conducted based on tumor (T) classification, lymph node (N) classification, and EBV DNA measurement to derive objectively the proposed stage groupings. The validity of the proposed stage groupings was confirmed in a prospective cohort of 550 consecutive patients who also received with IMRT.
Results
The pretreatment plasma EBV DNA level was identified as a significant, negative prognostic factor for progression‐free survival and overall survival in univariate analysis (all P < .001) and multivariate analysis (all P < .05). Recursive partitioning analysis of the primary cohort to incorporate EBV DNA generated the following proposed stage groupings: stage RI (T1N0), RIIA (T2‐T3N0 or T1‐T3N1, EBV DNA ≤2000 copies/mL), stage RIIB (T2‐T3N0 or T1‐T3N1, EBV DNA >2000 copies/mL; T1‐T3N2, EBV DNA ≤2000 copies/mL), stage RIII (T1‐T3N2, EBV DNA >2000 copies/mL; T4N0‐N2), and stage RIVA (any T and N3). In the validation cohort, the 5‐year progression‐free survival rate was 100%, 87.9%, 76.7%, 68.7%, and 50.4% for proposed stage RI, RIIA, RIIB, RIII, and RIV NPC, respectively (P < .001). Compared with the eighth edition TNM stage groupings, the proposed stage groupings incorporating EBV DNA provided better hazard consistency, hazard discrimination, outcome prediction, and sample size balance.
Conclusions
The proposed stage groupings have better prognostic performance than the eighth edition of the TNM staging system. EBV DNA titers should be included in the TNM staging system to assess patients who have EBV‐related NPC.
The proposed stage groupings incorporating Epstein‐Barr virus DNA by Recursive partitioning analysis have better prognostic performance than the eighth edition American Joint Committee on Cancer/Union for International Cancer Control TNM staging system. Compared with the eighth edition, the proposed stage groupings incorporating Epstein‐Barr virus DNA provide better hazard consistency, hazard discrimination, outcome prediction, and sample size balance
Hard carbon is regarded as a promising anode material for sodium‐ion batteries (SIBs). However, it usually suffers from the issues of low initial Coulombic efficiency (ICE) and poor rate performance, ...severely hindering its practical application. Herein, a flexible, self‐supporting, and scalable hard carbon paper (HCP) derived from scalable and renewable tissue is rationally designed and prepared as practical additive‐free anode for room/low‐temperature SIBs with high ICE. In ether electrolyte, such HCP achieves an ICE of up to 91.2% with superior high‐rate capability, ultralong cycle life (e.g., 93% capacity retention over 1000 cycles at 200 mA g−1) and outstanding low‐temperature performance. Working mechanism analyses reveal that the plateau region is the rate‐determining step for HCP with a lower electrochemical reaction kinetics, which can be significantly improved in ether electrolyte.
A self‐supporting, flexible, additive‐free and scalable hard carbon paper (HCP) derived from tissue is rationally developed, and it achieves outstanding Na‐storage properties in terms of high initial Coulombic efficiency (91.2%), superior high‐rate capability, ultralong cyclic stability, as well as outstanding low‐T performance in ether electrolyte. More significantly, the Na‐storage and capacity attenuation mechanism of the HCP anode is revealed.
Impossible voltage plateau regulation for the cathode materials with fixed active elemental center is a pressing issue hindering the development of Na‐superionic‐conductor (NASICON)‐type ...Na3V2(PO4)2F3 (NVPF) cathodes in sodium‐ion batteries (SIBs). Herein, a high‐entropy substitution strategy, to alter the detailed crystal structure of NVPF without changing the central active V atom, is pioneeringly utilized, achieving simultaneous electronic conductivity enhancement and diffusion barrier reduction for Na+, according to theoretical calculations. The as‐prepared carbon‐free high‐entropy Na3V1.9(Ca,Mg,Al,Cr,Mn)0.1(PO4)2F3 (HE‐NVPF) cathode can deliver higher mean voltage of 3.81 V and more advantageous energy density up to 445.5 Wh kg−1, which is attributed by the diverse transition‐metal elemental substitution in high‐entropy crystalline. More importantly, high‐entropy introduction can help realize disordered rearrangement of Na+ at Na(2) active sites, thereby to refrain from unfavorable discharging behaviors at low‐voltage region, further lifting up the mean working voltage to realize a full Na‐ion storage at the high voltage plateau. Coupling with a hard carbon (HC) anode, HE‐NVPF//HC SIB full cells can deliver high specific energy density of 326.8 Wh kg−1 at 5 C with the power density of 2178.9 W kg−1. This route means the unlikely potential regulation in NASICON‐type crystal with unchangeable active center becomes possible, inspiring new ideas on elevating the mean working voltage for SIB cathodes.
A high‐entropy effect is delicately introduced into fluorophosphate cathode for sodium‐ion batteries by in situ partial substitution of active V central atom, preparing a high‐entropy carbon‐free Na3V1.9(Ca,Mg,Al,Cr,Mn)0.1(PO4)2F3 cathode, suppressing the occurrence of detrimental phase transition process in the low‐voltage region, and further lifting up the mean working voltage of pristine Na3V2(PO4)2F3, enhancing sodium storage behavior, rate capability, and cycle performance.