摘要：The influence of the magnetism of transition metal oxide,nickel(II)oxide(NiO),on its surface reactivity and the dependence of surface reactivity on surface orientation and reactant magnetism were studied by density functional theory plus U *** considered five different antiferromagnetically ordered structures and one ferromagnetically ordered structure,NiO(001)and Ni(011)surfaces,paramagnetic molecule NO,and nonparamagnetic molecule *** calculations showed that the dependence of surface energies on magnetism was modest,ranging from49to54meV/?2for NiO(001)and from162to172meV/?2for NiO(011).On NiO(001),both molecules preferred the top site of the Ni cation exclusively for all NiO magnetic structures considered,and calculated adsorption energies ranged from?0.33to?0.37eV for CO and from?0.42to?0.46eV for *** NiO(011),both molecules preferred the bridge site of two Ni cations irrespective of the NiO *** was found that rather than the long‐range magnetism of bulk NiO,the local magnetic order of two coordinated Ni cations binding to the adsorbed molecule had a pronounced influence on *** calculated NO adsorption energy at the(↑↓)bridge sites ranged from?0.99to?1.05eV,and become stronger at the(↑↑)bridge sites with values of?1.21to?*** CO,although the calculated adsorption energies at the(↑↓)bridge sites(?0.73to?0.75eV)were very close to those at the(↑↑)bridge sites(?0.71to?0.72eV),their electron hybridizations were very *** present work highlights the importance of the local magnetic order of transition metal oxides on molecular adsorption at multi‐fold sites.

摘要：The development of cost-effective and highperformance electrocatalysts has been increasingly studied to mitigate upcoming energy and environmental *** and heterointerface engineering have played significant roles in the rational design of electrocatalysts and modulation of their electrocatalytic ***,the synergistic effect between amorphization and heterointerfaces has been scarcely *** a proof-of-concept attempt,we develop amorphous FeMo(a-FeMo)electrocatalysts with an abundance of heterointerfaces that are composed of amorphous components and evaluate their electrocatalytic performances toward the nitrogen reduction reaction and oxygen evolution reaction(OER).Benefitting from the synergistic effect between the amorphous nature of the a-FeMo electrocatalysts,which offer a high density of active sites,and significant electron redistribution at the heterointerfaces,the electrocatalysts exhibit a high Faradaic efficiency of 29.15%,an elevated yield rate of 71.78μg_(NH_(3)) mg_(cat.)^(-1) h^(-1) with long-term stability at a potential of-0.1V *** hydrogen electrode and excellent electrocatalytic activity toward the *** study provides a promising and effective method for the rational design of low-cost heterogeneous catalysts with desirable efficiency,selectivity,and stability.

摘要：The thermal conduction of suspended few-layer hexagonal boron nitride （h-BN） sheets was experimentally investigated using a noncontact micro-Raman spectroscopy method. The first-order temperature coefficients for monolayer （1L）, bilayer （2L） and nine-layer （9L） h-BN sheets were measured to be -（3.41 ± 0.12）× 10-2, -（3.15 ± 0.14） × 10-2 and -（3.78 ±0.16）× 10-2 cm-1.K-1, respectively. The room-temperature thermal conductivity of few-layer h-BN sheets was found to be in the range from 227 to 280 W.m-1-K-1, which is comparable to that of bulk h-BN, indicating their potential use as important components to solve heat dissipation problems in thermal management configurations.

摘要：Nanoporous metals show promising performances in electrochemical *** this paper,we report a self-supporting bimetallic porous heterogeneous indium/copper structure synthesized with a eutectic gallium-indium(EGaIn)material on a copper *** nanoporous copper-indium heterostructure catalyst exhibits excellent performance in the reduction of carbon dioxide to *** ratio of H_(2)/CO is tunable from 0.47 to 2.0 by changing working *** catalyst is highly stable,showing 96%maintenance of the current density after a 70-h continuous *** functional theory calculations reveal that the indium/copper interface induces charge redistribution within the copper surface,leading to the formation of two distinct active sites,namely,Cu^(δ)and Cu0,and enabling a high-performance generation of CO and H_(2).This work provides a new strategy for obtaining self-supporting nanoporous metal electrode catalysts.

摘要：As a clean and renewable future energy source, hydrogen fuel can be produced via solar water splitting. Two-dimensional (2D) black phosphorene (black-P) can harvest visible light due to the desirable band gap, which promises it as a metal-free photocatalyst. However, black-P can be only used to produce hydrogen since the oxidation potential of water locates lower than the position of the valence band maximum. To improve the photocatalytic performance of black-P, here, using black-P and blue phosphorene (blue-P) monolayers, we propose a 2D van der Waals (vdW) heterojunction. Theoretical results, including the band structures, density of states, Bader charge population, charge density di erence, and optical absorption spectra, clearly reveal that the visible light absorption ability is obviously improved, and the band edge alignment of the proposed vdW heterojunction displays a typical type-II feature to effectively separate the photogenerated carriers. At the same time, the built-in interfacial electric field prevents the electron-hole recombination. These predictions suggest that the examined phosphorene-based vdW heterojunction is an efficient photocatalyst for solar water splitting.

摘要：In contrast to heterogeneous network frameworks(e.g.,covalent organic frameworks and metal‐organic frameworks)and porous organic polymers,porous organic cages(POCs)are soluble molecules in common organic solvents that provide significant potential for homogeneous ***,we report a triphenylphosphine‐derived quasi‐porous organic cage(denoted as POC‐DICP)as an efficient organic molecular cage ligand for Rh/PPh_(3) system‐catalyzed homogeneous hydroformylation ***‐DICP not only displays enhanced hydroformylation selectivity(aldehyde selectivity as high as 97%and a linear‐to‐branch ratio as high as 1.89)but can also be recovered and reused via a simple precipitation method in homogeneous reaction *** speculate that the reason for the high activity and good selectivity is the favorable geometry(cone angle=123.88°)and electronic effect(P site is relatively electron‐deficient)of POC‐DICP,which were also demonstrated by density functional theory calculations and X‐ray absorption fine‐structure characterization.

摘要：The optoelectronic properties of atomically thin transition metal dichalcogenides(TMDs)are largely influenced by defect populations(DPs).In this work,we fabricate WSmonolayers with different DPs by varying the fabrication methods and further reveal their distinct exciton-exciton ***-state photoluminescence(PL)experiments show that the monolayer with the lowest DP shows optimal PL intensity at low excitation power;however,it is overtaken and significantly surpassed by monolayers with higher DPs at high excitation ***-power-dependent experiments demonstrate that these monolayers exhibit distinct PL saturation behaviors with the threshold power differing by four orders of *** with in situ PL imaging and time-resolved PL experiments,we attribute such PL evolution discrepancies to the different DPs within these monolayers,which largely influence the exciton diffusion behavior and subsequently bring about distinct nonradiative exciton-exciton annihilations(EEAs).Valley polarization experiments are further employed to re-examine the DPs of these *** work reveals the distinct PL behaviors and underlying exciton dynamics in TMD monolayers with different DPs,which can largely facilitate the engineering of relevant high-performance devices for practical applications.

摘要：The rational design and precise synthesis of multifunctional hybrid nanostructures with a tailored active core and a large, dendritic, modified mesoporous structured shell can promote catalysis, energy storage, and biological applications. Here, an oil-water biphase stratification coating strategy has been developed to prepare monodisperse magnetic dendritic mesoporous silica core-shell structured nano- spheres. These sophisticated Fe3O4@SiO2@dendritic-mSiO2 nanospheres feature large dendritic open pores （2.7 and 10.3 nm）. Significantly, the silica shells can be converted into dendritic mesoporous aluminosilicate frameworks with unchanged porosity, a Si/Al molar ratio of 14, and remarkably strong acidic sites, through a post-synthesis approach. In addition, the resultant magnetic dendritic mesoporous aluminosilicate nanospheres exhibit outstanding properties and promising application in phosphate removal from wastewater.

摘要：Heterostructure engineering holds exceptional promise for the development of high-performance electrocatalysts for overall water ***,production of inexpensive and high-efficiency bifunctional electrocatalysts remains a ***,we demonstrate a simple method to synthesize a paper-mulberry(Broussonetia papyrifera)-inspired Co_(9)S_(8)@CoNi_(2)S_(4)/nickel foam(Co_(9)S_(8)@CoNi_(2)S_(4)/NF)heterojunction with high catalytic activity and *** process involves in situ growth of NiCo layered double hydroxide and in situ derivatization of ZIF-67,followed by the S heteroatom *** Co_(9)S_(8)@CoNi_(2)S_(4)/NF benefits from the heterostructure and functional advantages of multidimensional building blocks including one-dimensional(1D)nanowires,2D nanosheets and *** optimized Co_(9)S_(8)@CoNi_(2)S_(4)/NF heterojunction with 10% sulphur content reveals excellent electrocatalytic activity with the lower overpotentials of 68 mV for hydrogen evolution reaction(HER)and 170 mV for oxygen evolution reaction(OER)at 10 mA cm^(-2) in the 1.0 mol L^(-1) KOH solution,which is superior to the recently reported transition metal based *** outstanding performance is attributed to the strong interface coupling between CoNi_(2)S_(4) and Co_(9)S_(8),the advantage of multidimensional structure and the customized electronic *** density functional theory suggests that the interface between Co_(9)S_(8) and CoNi_(2)S_(4) optimizes the adsorption of the multiple intermediates and further facilitates water splitting *** work offers a generic approach for heterostructure engineering design of highperformance catalytic system applications.

摘要：剪切增稠型聚硼硅氧烷(PBS)通常以“silly putty”,“bouncing putty”或“solid-liquid”被熟知.因其独特的抗冲击性能,PBS广泛应用于防护装甲、运动器材、玩具等领域.然而,自第二次世界大战PBS被发明后,PBS材料的更新升级较少.本论文中,我们通过设计联硼/氧配位键制备了一类新型剪切增稠材料——聚联硼硅氧烷(PDBS).结果表明,与单硼/氧配位键相比,联硼/氧配位键具有更多的配位结构和更高的键能,导致PDBS具有更类固体性的剪切增稠行为.因此,PDBS具有比PBS更优异的抗冲击性能与防护功能,为新一代智能装备、阻尼器和传感器的开发提供了一类高性能防护材料.