摘要：Due to their tunable acidity,shape selectivity,and excellent stability,zeolites are of great importance as solid acid materials in industrial *** the properties of the acid sites in zeolites allows for the rational design and fabrication of catalysts for target *** ether(DME)carbonylation,a critical chain-growth reaction for C1 resource utilization,is selectively catalyzed by the Brønsted acid sites within the eight-membered rings(8-MRs)of mordenite(MOR).It is anticipated that strengthening the Brønsted acidity—particularly in 8-MRs—will improve the catalytic performance of *** this work,density functional theory(DFT)calculations are first employed and the results used to design a modified MOR with stannum(Sn)and to predict the corresponding changes in *** by the theoretical studies,a series of Sn-modified MOR are synthesized via a defect-engineering and subsequent heteroatom-substitution *** partial desilication,isolated tetrahedral Sn species in an open configuration are successfully synthesized for the first time,within which tetrahedrally coordinated Al sites are *** acidic characterization is used to confirm that the acidity of the Brønsted acid sites is enhanced by the introduction of the Sn species;as a result,the sample exhibits excellent activity in DME carbonylation *** and DFT studies reveal that this strengthened acidity facilitates the adsorption of DME and reduces the activation barriers of DME dissociation and acetyl formation,accounting for the improved *** work demonstrates mechanistic insights into the promoting effects of strong acidity on DME carbonylation and offers a promising strategy to precisely control the acidic strength of zeolites.

摘要：Climate change caused by the increasing emission of CO_(2)to the atmosphere has become a global *** ameliorate this issue,converting CO_(2)into valuable chemicals is highly desirable,enabling a sustainable low-carbon *** this end,developing efficient catalytic systems for CO_(2)conversion has sparked intense interests from both academia and *** advantage of their highly porous structures and unique properties,metal−organic frameworks(MOFs)have shown great potential as heterogeneous catalysts for CO_(2)*** transformations involving CO_(2)have been accomplished over MOFs-based *** we provide a comprehensive and up-to-date review on recent advances of heterogeneous CO_(2)thermocatalysis using MOFs,highlighting relationships between structures and *** attention is given to the design strategies for improving the catalytic performance of *** available to enrich the catalytic active sites in MOF structures are stressed and their respective impacts on CO_(2)conversion efficiency are *** synergistic effects between each active site within the structure of MOFs and derivatives are *** the end,future perspectives and challenges in CO_(2)conversion by heterogeneous catalysis with MOFs are described.

摘要：Bio-nanochannels in living organisms participate in the physiological activities by selectively transporting ions through cell *** structure and function of biological ion channels inspire the development of artificial ion nanochannels with practical *** bioinspired nanochannels based on polymer materials present good mechanical stability,high-performance ion transport and designability,which have attracted much *** this review,we mainly focus on the fabrication and application of polymer-based biomimetic nanochannels especially in environmentally responsive biosensor and energy *** firstly introduce the basic understanding of nanochannels in ion regulation and osmotic energy ***,we discuss the fabrication methods of polymer-based nanochannels and highlight their advantages compared with other *** practical applications of polymer-based biomimetic nanochannels,especially in energy conversion and environmentally responsive biosensor,are detailedly ***,we summarize the unsolved problems in bioinspired nanochannels and overview the further developing direction in this field.

摘要：Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from low *** this article,we report a tractable approach to modifying g-C3N4 with vanadyl phthalocyanine(VOPc/CN)for efficient visible-light-driven hydrogen production.A non-covalent VOPc/CN hybrid photocatalyst formed viaπ-πstacking interactions between the two components,as confirmed by analysis of UV-vis absorption *** VOPc/CN hybrid photocatalyst shows excellent visible-light-driven photocatalytic performance and good *** optimal conditions,the corresponding H2 evolution rate is nearly 6 times higher than that of pure *** role of VOPc in promoting hydrogen evolution activity was to extend the visible light absorption range and prevent the recombination of photoexcited electron-hole pairs *** is expected that this facile modification method could be a new inspiration for the rational design and exploration of g-C3N4-based hybrid systems with strong light absorption and high-efficiency carrier separation.

摘要：Owing to the excellent redox reversibility and structural diversity,polytriphenylamine(PTPAn)has been regarded as one of the promising cathode candidates for sodium-ion ***,it still suffers from the bulk aggregation and low operating capacity in practical *** by the in-situ polymerization,leaf-like PTPAn nanosheets are uniformly introduced on the surface of carbon nanofibers(CNFs)to form the free-standing CNF@PTPAn composite ***,the formation mechanism of the leaf-on-branch structure of CNF@PTPAn composites is systematically explored,confirming that the controlling of oxidation rate and growth degree plays crucial roles in tuning the morphology and active material content of the composite *** by the capacity-cutting analysis,the effective coupling between the active PTPAn and conductive CNFs can provide fast electron/ion-shuttling channels and deepen the electrochemical reaction *** 50mAg^(-1),the capacity of the optimized CNF@PTPAn composite can reach 105mAh g^(-1),with a stable rate capability of 78mAh g^(-1)even at 400mAg^(-1)after 500 cycles in a half *** detailed kinetic analysis confirms that the ion-storage behaviors in the lowvoltage region can be tailored for the improved capacitive contribution and diffusion ***,the flexible CNF-based full cell with CNF@PTPAn as the cathode and CNFs as the anode exhibits a high energy density of 60Wh kg^(-1)at 938Wkg^(-1).Based on this,the rational design is expected to provide more possibilities to obtain advanced freestanding electrode systems.

摘要：Due to their unique surface chemistry,highly adjustable metal components,hydrophilicity,and high carrier concentrations,MXenes are applied in a variety of *** to other two-dimensional(2D)materials,building heterostructures with additional materials to form a 3D porous architecture for MXenes can significantly enhance their functionality and ***,the open structures and well-defined pathways of these 3D structured MXenes can improve ionic and electronic transport,thereby promoting their applications in electrochemical energy storage,sensing,catalysis,and *** this review,the recent efforts made on preparing 3D porous MXenes with heterostructures,focusing on MXenes/C,MXenes/inorganics,and MXenes/polymers were *** discussion covers aspects ranging from the design to synthesis of 3D porous MXenes,and their applications in photocatalysis,environmental monitoring and electrochemical energy *** review is concluded by presenting the prospects and insights on exploring the relationships between the porosity formation mechanisms,properties and applications of the 3D porous MXenes *** review can provide meaningful guidance for the design,fabrication and application of 3D porous MXenes in high-performance materials and devices.

摘要：Owing to its photonic band gap(PBG)and slow light effects,aniline black(AB)-poly(vinylidene fluoride)(PVDF)inverse opal(IO)photonic crystal(PC)was constructed to promote the utility of light and realize photothermal synergetic *** a highly efficient reaction platform with the capability of restricting heat,a microreactor was introduced to further amplify the photothermal effects of near infrared(NIR)*** photocatalytic efficiency of ZnO/0.5AB-PVDF IO(Z0.5A)increases 1.63-fold compared to that of pure ZnO film under a full solar spectrum,indicating the effectiveness of synergetic promotion by slow light and photothermal ***,a 5.85-fold increase is achieved by combining Z0.5A with a microreactor compared to the film in a *** photon localization effect of PVDF IO was further exemplified by finite-difference time-domain(FDTD)*** conclusion,photonic crystal-microreactor enhanced photothermal catalysis has immense potential for alleviating the deteriorating water environment.

摘要：Recurrent oral ulcer is a painful oral mucosal disorder that affects 20%of the world’s *** lack of a radical cure due to its unknown underlying cause calls for innovative symptomatic *** work reports a hyaluronic acid-based dissolvablemicroneedle patch(ROUMNpatch,short for recurrent oral ulcer microneedle)loaded with dexamethasone acetate,vitamin C and tetracaine hydrochloride for the treatment of recurrent oral *** ROUMN patch shows enhancement in both the anti-inflammatory effect elicited by dexamethasone and the pro-proliferation effect of vitamin *** vitro experiments show that ROUMN has a higher efficiency in suppressing lipopolysaccharide(LPS)-induced interleukin-6(IL-6)expression than dexamethasone *** proliferation and migrationwere also significantly promoted byROUMNcompared to vitamin C *** healing-promoting effect of ROUMN was also verified in vivo using an acetic acid-cauterized oral ulcer model in *** as a treatment accelerated the healing process of oral ulcers,shortening the total healing time to 5 days compared with the 7 days required by treatment using watermelon frost,a commonly used over-the-counter(OTC)drug for oral *** rapid dissolution of the hyaluronic acid-based microneedles and the superior healing-promoting effect of the drug combination could lead to a broad application prospect of the ROUMN patch in the treatment of recurrent oral ulcers.

摘要：Heterogeneous molecular catalysts,such as metal phthalocyanines,are efficient electrocatalysts for CO_(2) reduction reaction(CO_(2)RR).However,the rational design and synthesis of a molecular catalyst-based heterostructure for CO_(2)RR remains ***,we developed a crystalline bimetallic phthalocyanine heterostructure electrocatalyst(CoPc/FePc HS),which achieved an excellent CO_(2)-to-CO conversion efficiency(99%)and outstanding long-term stability after 10 h of *** functional theory calculations revealed that the enhancement of CO_(2)RR performance could be attributed to the distinct electron transfer pattern between FePc and *** heterostructural engineering in molecular catalysts would inspire a unique approach for improving CO_(2)RR performance.

摘要：Modulating the extracellular matrix microenvironment is critical for achieving the desired macrophage phenotype in immune investigations or tumor *** de novo protein design and biosynthesis techniques,herein,we designed a biomimetic polypeptide self-assembled nano-immunomodulator to trigger the activation of a specific macrophage *** was intended to be made up of(GGSGGPGGGPASAAANSASRATSNSP)n,the RGD motif from collagen,and the IKVAV motif from *** combination of these domains allows the biomimetic polypeptide to assemble into extracellular matrix-like nanofibrils,creating an extracellular matrix-like milieu for ***,changing the concentration further provides a facile route to fine-tune macrophage polarization,which enhances antitumor immune responses by precisely resetting tumor-associated macrophage immune responses into an M1-like phenotype,which is generally considered to be tumor-killing macrophages,primarily antitumor,and *** metal or synthetic polymer-based nanoparticles,this polypeptide-based nanomaterial exhibits excellent biocompatibility,high efficacy,and precise tunability in immunomodulatory *** encouraging findings motivate us to continue our research into cancer immunotherapy applications in the future.