摘要：Electrochemical CO_(2)reduction reaction(CO_(2)RR)driven by sustainable energy has emerged as an attractive route to achieve the target of carbon *** is one of the most economically viable products,and electrocatalytic CO_(2)RR to formate is a promising ***-pressure H-cell electrolyzer is easy to operate and allows high CO_(2)solubility for realizing high current density,but the design of highly efficient catalysts for working under high CO_(2)pressures remains ***-based catalysts exhibit high formate selectivity,but suffer from limited ***,we report a high-performance catalyst,which is derived from BiPO_(4)nanopolyhedrons during electrocatalytic CO_(2)RR to formate in neutral solution under high CO_(2)pressures.A high partial current density of formate(534 mA cm^(−2))and formate formation rate(9.9 mmol h^(−1) cm^(−2))with a formate Faradaic efficiency of 90%have been achieved over BiPO_(4)-derived catalyst at an applied potential of−0.81 V *** under 3.0 MPa CO_(2)*** discover that BiPO_(4)nanopolyhedrons evolve into metallic Bi nanosheets with rich grain boundaries in electrocatalytic CO_(2)RR under high CO_(2)pressures,and the grain boundaries of the BiPO_(4)-derived catalyst play a vital role in promoting electrocatalytic CO_(2)RR to *** theoretical studies reveal that the charge redistribution occurs at the grain boundaries of Bi surface,and this promotes CO_(2)activation and increases HCOO^(*)intermediate stability,thus making the pathway for CO_(2)RR to formate more selective and *** work not only demonstrates a highly efficient catalyst for CO_(2)RR to formate but also discovers a unique feature of catalyst evolution under high CO_(2)pressures.

摘要：Chemically modified carbonaceous materials have attained utmost attention in the fields of renewable energy storage and conversion,due to the controllable physicochemical properties,tailorable micro-/nanostructures,and respectable ***,P-doped mesoporous carbons were synthesized by using F127 as the soft template,organophosphonic acid as the P source and phenolic resin as the carbon *** amounts of iron species were introduced to act as a graphitization *** synthesized carbons exhibit the well-defined wormhole-like pore structure featuring high specific surface area and homogenously doped P ***,introducing iron species during the synthesis process can optimize the textural properties and the degree of graphitization of carbon *** doping amount of P has an important effect on the porous structure and the defect degree,which correspondingly influence the active sites and the oxygen reduction reaction(ORR)*** resultant material presents superior catalytic activity for the ORR,together with remarkably enhanced durability and methanol tolerance in comparison with the commercial Platinum catalyst,demonstrating the possibility for its use in electrode materials and electronic nanodevices for metal-air batteries and fuel cells.

摘要：Rechargeable Li batteries as electrochemical energy storage and conversion devices are continuously changing human life. In order to meet the increasing demand for energy and power density, it is essential and urgent to exploit the electrode materials with high capacity and fast charge transfer(for Li-ion and Li-S batteries) and electrocatalysts with high activity(for rechargeable Li-O2 batteries). The high capacity is attributed to high electron transfer number and low molecular weight of the electrode materials. Combined with proper nanostructure design, the electronic transfer and ionic conductivity will be improved. This review summarizes recent efforts to apply electrode materials for Li-ion batteries with multi-electron reaction, Li-S batteries, and efficient electrocatalysts for Li-O2 batteries. The methods to enhance the cycling and rate performance have been discussed in detail. Advanced rechargeable Li batteries with multi-electron reaction will become the research emphasis in the future.

摘要：A Z-scheme is a promising approach to achieve broad-spectrum photocatalysis. Integration of TiO2 with another semiconductor with a band gap of -1.0 eV would be ideal to harvest both ultraviolet and visible-near infrared light for photocatalysis; however, most narrow-bandgap semiconductors have straddling band structure alignments with TiO2, constituting an obstacle to forming the Z-scheme for photocatalytic hydrogen production. In this communication, we demonstrate Ag2S as a model system where the energy band upshift of the narrow-bandgap semiconductor that shares an interface with a metal can overcome this limitation. To fabricate the design, we developed a unique approach to synthesize Ag2S-Ag-TiO2 hybrid structures. The obtained ternary hybrid structures exhibited dramatically enhanced performance in photocatalytic hydrogen pro- duction under full-spectrum light illumination. The activities were significantly higher than the sum of those of Ag2S-Ag-TiO2 structures under λ〈 400 nm and λ 〉 400 nm irradiation as well as those of their counterparts under any light illumination conditions.

摘要：Reverse water gas shift（RWGS） reaction can be served as a pivotal stage of transitioning the abundant CO;resource into chemicals or hydrocarbon fuels, which is attractive for the CO;utilization and of eventually significance in enabling a rebuilt ecological system for unconventional fuels. This concept is appealing when the process is considered as a solution for the storage of renewable energy, which may also find a variety of potential end uses for the outer space exploration. However, a big challenge to this issue is the rational design of high temperature endurable RWGS catalysts with desirable CO product selectivity. In this work, we present a comprehensive overview of recent publications on this research topic,mainly focusing on the catalytic performance of RWGS reaction over three major kinds of heterogeneous catalysts, including supported metal catalysts, mixed oxide catalysts and transition metal carbides. The reaction thermodynamic analysis, kinetics and mechanisms are also described in detail. The present review attempts to provide a general guideline about the construction of well-performed heterogeneous catalysts for the RWGS reaction, as well as discussing the challenges and further prospects of this process.

摘要：In this work, the intra-EDA method, which is a recently developed energy decomposition analysis scheme for intramolecular non-covalent interaction is extended from gas phase to solvated environment. It is the first analysis scheme that performs analysis for intramolecular interaction in solution. By fragmentation scheme, a molecule is divided into intramolecular interacting fragments and environmental fragments via single bond homolysis breaking. The solvent effect is taken into account by implicit solvation model. Intramolecular interaction free energy is estimated as the separated treatment of inter-fragment interactions in dielectric environment. The analysis results highlight the importance of solvent effects to intramolecular non-covalent interaction.

摘要：Recent studies confirm that the emerging bifunctional catalysts consisting of metal oxide and zeolites can directly convert syngas into high-quality gasoline,however,the formation mechanism of iso-paraffins and the difference with the conventional FT/zeolite catalyst have not been ***,three one-dimensional SAPO zeolites with diverse micropore sizes were synthesized and assembled with ZnAlO_(x)with spinel *** was found that ZnAlO_(x)/SAPO-41 and ZnAlO_(x)/SAPO-11 with medium micropore sizes favored the formation of C_(5)–C_(11)hydrocarbons with a high content of *** characterizations pointed out that the formation of iso-paraffins over SAPO-11 followed a pore-mouth catalysis mechanism,which means the isomerization of linear hydrocarbons can only take place near the pore mouth region of *** mechanism only allows the formation of mono-branched iso-paraffins in the C_(5)–C_(11)range,which are less prone to be cracked than their di-branched isomers.A careful comparative analysis between ZnAlO_(x)/SAPO-11 and Co/H-meso-ZSM-5 was also made in terms of product distribution,activity,and stability.

摘要：The binding energy and generalized stacking-fault energy (GSFE) are two critical interface properties of two dimensional layered materials, and it is still unclear how neighboring layers affect the interface energy of adjacent layers. Here, we investigate the effect of neighboring layers by comparing the differences of binding energy and GSFE between trilayer heterostructures (graphene/graphene/graphene, graphene/graphene/boron nitride,boron nitride/graphene/boron nitride) and bilayer heterostructures (graphene/graphene,graphene/boron nitride) using density functional theory. The binding energy of the adjacent layers changes from -2.3% to 22.55% due to the effect of neighboring layer, with a very small change of the interlayer distance. Neighboring layers also make a change from -2% to 10% change the GSFE, depending on the property of the interface between adjacent layers. In addition, a new simple expression is proven to describe the GSFE landscape of graphene-like structure with high accuracy.

摘要：Alloying Pt with transition metals can significantly improve the catalytic properties for the oxygen reduction reaction(ORR).However,the application of Pt-transition metal alloys in fuel cells is largely limited by poor long-term durability because transition metals can easily *** this study,we developed a nonmetallic doping approach and prepared a P-doped Pt catalyst with excellent durability for the ***-supported core-shell nanoparticles with a P-doped Pt core and Pt shell(denoted as PtPx@Pt/C)were synthesized via heat-treatment phosphorization of commercial Pt/C,followed by acid *** analysis using electron energy loss spectroscopy and X-ray photoelectron spectroscopy clearly demonstrated that Pt was enriched in the near-surface region(approximately 1 nm)of the carbon-supported core-shell *** to P doping,the ORR specific activity and mass activity of the PtP_(1.4)@Pt/C catalyst were as high as 0.62 mA cm^(–2)and 0.31 mAμgPt–^(1),respectively,at 0.90 V,and they were enhanced by 2.8 and 2.1 times,respectively,in comparison with the Pt/C *** importantly,PtP_(1.4)@Pt/C exhibited superior stability with negligible mass activity loss(6%after 30000 potential cycles and 25%after 90000 potential cycles),while Pt/C lost 46%mass activity after 30000 potential *** high ORR activity and durability were mainly attributed to the core-shell nanostructure,the electronic structure effect,and the resistance of Pt nanoparticles against aggregation,which originated from the enhanced ability of the PtP_(1.4)@Pt to anchor to the carbon *** study provides a new approach for constructing nonmetal-doped Pt-based catalysts with excellent activity and durability for the ORR.

摘要：Transition metal nitrides （TMNs） are of particular interest by virtue of their synergic advantages of superior electrical conductivity, excellent environmental durability and high reaction selectivity, yet it is difficult to achieve flexible design and operation. Herein, mesocrystal nanosheets （MCNSs） of vanadium nitride （VN） are synthesized via a confined-growth route from thermally stable layered vanadium bronze, representing the first two-dimensional （2D） metallic mesocrystal in inorganic compounds. Benefiting from their single-crystalline-like long-range electronic connectivity, VN MCNSs deliver an electrical conductivity of 1.44×10^5 S/m at room temperature, among the highest values observed for 2D nanosheets. Coupled with their unique pseudocapacitance, VN MCNS-based flexible supercapacitors afford a superior volumetric capacitance of 1,937 mF/cm3. Nitride MCNSs should have wide applications in the energy storage and conversion fields because their intrinsic high conductivity is coupled with the reactivity of inorganic lattices.