Cu_(3)P辅助诱导Ni_(2)P电荷定向转移和表面重构以获得高效析氧活性

与助催化剂形成异质结,通过调整活性位点的电子结构和电荷输运来提高Ni_(2)P的电催化活性是一种可行的方法。本文成功构建了一种高效的Cu_(3)P/Ni_(2)P异质结催化剂,其中Cu_(3)P本身仅作为助催化剂,通过调节Ni_(2)P的电子转移和表面重构来提高电催化活性。结果表明,在10 mA·cm^(-2)的电流密度下,Cu_(3)P/Ni_(2)P具有优异的析氧反应(OER)活性,过电位为213 mV。结合实验结果和理论计算可知,Cu_(3)P助催化剂可以有效调整Ni中心的电子结构,实现电荷重分布,降低反应能垒,从而显著提高OER催化活性。此外,Cu_(3)P助催化剂诱导的丰富的晶界和晶格畸变促进了表面重构,形成Ni5O(OH)9,为OER提供了有效的活性位点。本工作通过引入助催化剂构建了一种新型异质结电催化剂,为优化过渡金属磷化物的电催化性能提供了一条有效途径。

Simulating the evolution of focused waves by a two-layer Boussinesq-type model

Accurate simulation of the evolution of freak waves by the wave phase focusing method requires accurate linear and nonlinear properties,especially in deep-water conditions.In this paper,we analyze the ability to simulate deep-water focused waves of a two-layer Boussinesq-type(BT)model,which has been shown to have excellent linear and nonlinear performance.To further improve the numerical accuracy and stability,the internal wavegenerated method is introduced into the two-layer Boussinesq-type model.Firstly,the sensitivity of the numerical results to the grid resolution is analyzed to verify the convergence of the model;secondly,the focused wave propagating in two opposite directions is simulated to prove the symmetry of the numerical results and the feasibility of the internal wave-generated method;thirdly,the limiting focused wave condition is simulated to compare and analyze the wave surface and the horizontal velocity of the profile at the focusing position,which is in good agreement with the measured values.Meanwhile the simulation of focused waves in very deep waters agrees well with the measured values,which further demonstrates the capability of the two-layer BT model in simulating focused waves in deep waters.

A GPU accelerated Boussinesq-type model for coastal waves

This study presents an efficient Boussinesq-type wave model accelerated by a single Graphics Processing Unit(GPU).The model uses the hybrid finite volume and finite difference method to solve weakly dispersive and nonlinear Boussinesq equations in the horizontal plane,enabling the model to have the shock-capturing ability to deal with breaking waves and moving shoreline properly.The code is written in CUDA C.To achieve better performance,the model uses cyclic reduction technique to solve massive tridiagonal linear systems and overlapped tiling/shared memory to reduce global memory access and enhance data reuse.Four numerical tests are conducted to validate the GPU implementation.The performance of the GPU model is evaluated by running a series of numerical simulations on two GPU platforms with different hardware configurations.Compared with the CPU version,the maximum speedup ratios for single-precision and double-precision calculations are 55.56 and 32.57,respectively.

A Central Numerical Scheme to 1D Green-Naghdi Wave Equations

A numerical scheme based on hybrid central finite-volume and finite-difference method is presented to model Green-Naghdi water wave equations. The governing equations are reformulated into the conservative form, and the convective flux is estimated using a Godunov-type finite volume method while the remaining terms are discretized using finite difference method. To enhance the robustness of the model, a central-upwind flux evaluation and a well-balanced non- negative water depth construction are incorporated. Numerical tests demonstrate that present model has the advantages of stability preserving and numerical efficiency.

Synergy of phosphorus vacancies and build-in electric field into NiCo/NiCoP Mott-Schottky integrated electrode for enhanced water splitting performance

Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer,regulate adsorption energy of reaction intermediates,and provide additional active sites,which are regarded as valid means for improving catalytic activity.However,the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains unclear.Herein,the growth of a bifunctional NiCo/NiCoP Mott-Schottky electrode with abundant phosphorus vacancies on foam nickel(NF)has been synthesized through continuous phosphating and reduction processes.The obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities,and the overpotentials for OER and HER are as low as 117 and 60 mV at 10 mA/cm^(2) in 1 mol/L KOH,respectively.Moreover,as both the cathode and anode of overall water splitting,the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10 mA/cm^(2),which are far exceeding the benchmark commercial electrodes.DFT theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor,tailor the electronic structure of the metal centers and lower the Gibbs free energy of the intermediates.Furthermore,the unique self-supported integrated structure is beneficial to facilitate the exposure of the active site,avoid catalyst shedding,thus improving the activity and structural stability of NiCo/NiCoP.This study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.

Interfacial charge redistribution to promote the catalytic activity of Vs-CoP-CoS_(2)/C n-n heterojunction for oxygen evolution

Modulating surface charge redistribution based on interface and defect engineering has been considered as a resultful means to boost electrocatalytic activity.However,the mechanism of synergistic regulation of heterojunction and vacancy defects remains unclear.Herein,a Vs-CoP-CoS_(2)/C n-n heterojunction with sulfur vacancies is successfully constructed,which manifests superior electrocatalytic activity for oxygen evolution,as demonstrated by a low overpotential of 170 mV to reach 10 mA/cm^(2).The experimental results and density functional theory calculations testify that the outstanding OER performance of Vs-CoP-CoS_(2)/C heterojunction is owed to the synergistic effect of sulfur vacancies and built-in electric field at n-n heterogeneous interface,which accelerates the electron transfer,induces the charge redistribution,and regulates the adsorption energy of active intermediates during the reaction.This study affords a promising means to regulate the electrocatalytic performance by the construction of heterogeneous interfaces and defects,and in-depth explores the synergistic mechanisms of n-n heterojunction and vacancies.

Facile fabrication of self-healing silicone-based poly(urea-thiourea)/tannic acid composite for anti-biofouling

A novel silicone-based poly(urea-thiourea)/tannic acid composite(PDMS-P(Ua-TUa)-TA)with excellent mechanical,self-healing and antifouling properties is developed.The multiple dynamic hydrogen bonds formed by thiourea groups,urea groups,and tannic acid(TA)molecules ensured a tough elastomer(ultimate strength:2.47 MPa)with high stretchability(~1000%).TA molecules as partial hydrogen bonding cross-linking sites interacted rapidly with urea and thiourea groups before the migration of polymer chains,resulting in fast and efficient self-healing.Scratches on the film completely disappeared within12 min,and the repair efficiency of strength was up to 98.4%within 3 h under ambient condition.Selfhealing behavior was also evaluated in artificial seawater and the healing efficiency(HE)was 95.1%.Furthermore,TA uniformly dispersed in the polymer matrix provides good antibacterial and anti-diatom properties,as well as strong adhesion to the substrate(~2.2 MPa).Laboratory bioassays against marine bacteria adhesion(~96%,~95%and~93%reduction for P.sp.,E.coli,and S.aureus,respectively)and diatom attachment(~84%reduction)demonstrated an outstanding antifouling property of the PDMSP(Ua-TUa)-TA.This work provides a promising pathway towards the development of high-performance silicone-based coatings for marine anti-biofouling.

Co-Construction of Sulfur Vacancies and Heterogeneous Interface into Ni_(3)S_(2)/MoS_(2) Catalysts to Achieve Highly Efficient Overall Water Splitting

Integrating the advantages of anion vacancies and heterostructures into the catalytic materials may increase the binding affinities to intermediates, provide more active sites, and significantly promote the activity of overall water splitting. However, the successful assembly of anion vacancies and heterostructures for high-efficiency water splitting performance is still challenging. In this work, we ingeniously present the co-construction of sulfur vacancies and heterogeneous interface into Ni_(3)S_(2)/MoS_(2) catalysts on nickel foam(NF). The introduction of sulfur vacancies and Ni_(3)S_(2)/MoS_(2) heterostructures can significantly improve electron and ion transport, effectively improve structural stability, and enhance overall water splitting activity. The obtained VSNi_(3)S_(2)/MoS_(2) catalysts(VS stands for sulfur vacancies) exhibit superior OER and HER activities,and the overpotentials for OER and HER are 180 and 71 mV at 10 mA·cm^(-2), respectively. Furthermore, a low water splitting voltage of 1.46 V is required at 10 mA·cm^(-2) for the VS-Ni_(3)S_(2)/MoS_(2) catalysts, which is considerably lower than most that of water splitting electrocatalysts currently reported. This work offers an effective mean for the preparation of catalysts with both anion vacancies and heterostructures for achieving high-performance alkaline overall water splitting.

Flexible Organic Single Crystal with Elastic Bending and Plastic Twisting Capabilities

INTRODUCTION Organic single crystals have found wide-spread applications in smart materials,[1]optical waveguide devices,[2]photonic applications,[3]lasers,[4]OLED materials,and so on.