摘要：Aqueous hybrid supercapacitors(AHSCs)offer potential safety and eco-friendliness compared with conventional electrochemical energy storage devices that use toxic and flammable organic *** can serve as the bridge between aqueous batteries and aqueous supercapacitors by combining the advantages of high energy of the battery electrode and high power as well as long lifespan of the capacitive *** the past few decades,extensive research efforts have been devoted to developing advanced materials and fascinating device architectures for ***,further development related to the compatibilities between the battery-type electrode and capacitive electrode remains stagnant mainly due to discrepancy encountered in terms of reaction kinetics and *** review focuses on the recent progress made in the field of AHSCs via elucidating the main concepts on the design of battery and capacitive electrodes and emerging *** particular,ingenious AHSCs that possess either better flexibility toward materials selection or better device functionality such as those with“dual-ion”energy storage mechanism and non-polarity feature are also *** advances and unresolved issues in multivalent ion hybrid devices(in particular,zinc-ion AHSCs)are further ***,future research directions and challenges for AHSCs are presented,which are anticipated to deliver higher energy and demonstrate greater multifunctionalities for more breakthrough technology applications.

摘要：Conjugated covalent organic frameworks(COFs)hold great promise in photocatalytic hydrogen evolution owing to their high crystallinity,large surface area,and distinct ***,COFs exhibit poor charge ***,investigating highly effective COF-based photocatalysts is *** the first time,conjugated COF/perylene diimide urea polymer(PUP)all-organic heterostructure with S-scheme interfacial charge-transfer channels was successfully developed and manufactured via in situ coupling of the two-dimensional triazine-based imine-linked COF(denoted as TATF-COF)with *** optimal photocatalytic hydrogen-evolution rate of 94.5 mmol h^(-1) g^(-1) for TATF-COF/PUP is 3.5 times that of pure TATF-COF and is comparable to or even higher than that of the previously reported COF-based photocatalysts,resulting in an apparent quantum efficiency of up to 19.7%at 420 *** improved directional S-scheme charge transfer driven by the tuned built-in electric field and enhanced oxidation and reduction reaction rates of the photogenerated carriers contribute synergistically to the boosted photocatalytic H_(2) *** and theoretical studies reveal plausible H_(2) evolution and spatial S-scheme charge-separation mechanisms under visible-light *** study provides advanced methods for constructing all-organic S-scheme high-efficiency photocatalysts by the modulation of band structures.

摘要：Inspired by MXene nanosheets and their regulation of surface functional groups,a series of Ti_(2)C‐based single‐atom electrocatalysts(TM@Ti_(2)CT_(x),TM=V,Cr,Mn,Fe,Co,and Ni)with two dif‐ferent functional groups(T=–O and–S)was *** CO_(2)RR catalytic performance was stud‐ied using well‐defined ab initio *** results show that the CO_(2) molecule can be more readily activated on TM@Ti_(2)CO_(2) than the TM@Ti_(2)CS_(2) *** charge analysis reveals that the Ti_(2)CO_(2) substrate is involved in the adsorption reaction,and enough electrons are injected into the 2π*u orbital of CO_(2),leading to a V‐shaped CO_(2) molecular configuration and partial negative charge *** V‐shaped CO_(2) further reduces the difficulty of the first hydrogenation reac‐tion *** calculatedΔG of the first hydrogenation reaction on TM@Ti_(2)CO_(2) was significantly lower than that of the TM@Ti_(2)CS_(2) ***,the subsequent CO_(2) reduction pathways show that the UL of the potential determining step on TM@Ti_(2)CS_(2) is smaller than that of TM@Ti_(2)CO_(2).Combining the advantages of both TM@Ti_(2)CS_(2) and TM@Ti_(2)CO_(2),we designed a mixed functional group surface with–O and–S to anchor TM *** results show that Cr atoms an‐chored on the surface of mixed functional groups exhibit high catalytic activity for the selective production of *** study opens an exciting new avenue for the rational design of highly selec‐tive MXene‐based single‐atom CO_(2)RR electrocatalysts.

摘要：Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined *** tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past *** substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently ***,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed ***,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are *** particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.

摘要：Cadmium sulfide(Cd S)-based photocatalysts have attracted extensive attention owing to their strong visible light absorption,suitable band energy levels,and excellent electronic charge transportation *** review focuses on the recent progress related to the design,modification,and construction of Cd S-based photocatalysts with excellent photocatalytic H2 evolution ***,the basic concepts and mechanisms of photocatalytic H2 evolution are briefly ***,the fundamental properties,important advancements,and bottlenecks of Cd S in photocatalytic H2 generation are presented in detail to provide an overview of the potential of this ***,various modification strategies adopted for Cd S-based photocatalysts to yield solar H2 are discussed,among which the effective approaches aim at generating more charge carriers,promoting efficient charge separation,boosting interfacial charge transfer,accelerating charge utilization,and suppressing charge-induced *** critical factors governing the performance of the photocatalyst and the feasibility of each modification strategy toward shaping future research directions are comprehensively discussed with ***,the prospects and challenges encountered in developing nanostructured Cd S and Cd S-based nanocomposites in photocatalytic H2 evolution are presented.

摘要：The development of highly active DFT catalysts for an electrocatalytic N_(2)reduction reaction(NRR)under mild conditions is a difficult *** this study,a series of atom‐pair catalysts(APCs)for an NRR were fabricated using transition‐metal(TM)atoms(TM=Sc−Zn)doped into g‐CN *** electrochemical mechanism of APCs for an NRR has been reported by well‐defined density functional theory *** calculated limiting potentials were−0.47 and−0.78 V for the Fe_(2)@CN and Co_(2)@CN catalysts,*** to its high suppression of hydrogen evolution reactions,Co_(2)@CN is a superior electrocatalytic material for a N_(2)*** Fe_(2)@CN may be a strongly attractive material for an NRR with a relatively low overpotential after an improvement in the *** two‐way charge transfer affirmed the donation‐acceptance procedure between N_(2)and Fe_(2)@CN or Co_(2)@CN,which play a crucial role in the activation of inert N≡N *** study provides an in‐depth investigation into atom‐pair catalysts and will open up new avenues for highly efficient g‐CN‐based nanostructures for an NRR.

摘要：The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very *** this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple ***-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid *** apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,***,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole ***,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic *** study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.