Accelerating the Screening of Modified MA_(2)Z_(4) Catalysts for Hydrogen Evolution Reaction by Deep Learning-Based Local Geometric Analysis

Machine learning(ML)integrated with density functional theory(DFT)calculations have recently been used to accelerate the design and discovery of single-atom catalysts(SACs)by establishing deep structure–activity relationships.The traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods,leading to the limitation of the potential application range.Aiming to the structural properties of several typical two-dimensional MA_(2)Z_(4)-based single-atom systems(bare MA_(2)Z_(4) and metal single-atom doped/supported MA_(2)Z_(4)),an improved crystal graph convolutional neural network(CGCNN)classification model was employed,instead of the traditional machine learning regression model,to address the challenge of incompatibility in the studied systems.The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer,surface layer,and bulk layer(ASB-GCNN).Through ML and DFT calculations,five potential single-atom hydrogen evolution reaction(HER)catalysts were screened from chemical space of 600 MA_(2)Z_(4)-based materials,especially V_(1)/HfSn_(2)N_(4)(S)with high stability and activity(Δ_(GH*)is 0.06 eV).Further projected density of states(pDOS)analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-dz^(2)orbital coincided with the H-s orbital around the energy level of−2.50 eV,and orbital analysis confirmed the formation ofσbonds.This study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.

Effect of ZrC Modified Graphite on Structure and Properties of Low-carbon Al_(2)O_(3)-C Refractories

To address the issues of reduced performance and shortened lifespan during the low-carbonizating process of Al_(2)O_(3)-C refractories,nano-crystalline ZrC modified graphite was prepared using Zr powder and flake graphite as raw materials,with NaCl and NaF mixed salt serving as the medium.The flake graphite was gradually replaced by ZrC modified graphite in the preparation of Al_(2)O_(3)-C refractories,and its impact on the material’s structure and properties was investigated.The results indicate that,compared to samples with only flake graphite,the introduction of 1 mass%to 5 mass%nano-crystalline ZrC modified graphite can significantly enhance the mechanical performance of low-carbon Al_(2)O_(3)-C refractories.When 5 mass%ZrC modified graphite is added,the mechanical properties of the samples are optimal,with the cold modulus of rupture and elastic modulus reaching 22.5 MPa and 65.0 GPa,respectively.

Exploring the impact of Nafion modifier on electrocatalytic CO_(2) reduction over Cu catalyst

Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)electrolysis.Herein,the key roles of Nafion for CO_(2)RR were systematically studied on Cu nanoparticles(NPs)electrocatalyst.We found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H_(2)O from electrolyte to Cu NPs,and increase the CO_(2)concentration at electrocatalyst interface for enhancing the CO_(2)mass transfer process,but also activate CO_(2)molecule by Lewis acid-base interaction between Nafion and CO_(2)to accelerate the formation of^(*)CO,which favor of C–C coupling for boosting C_(2)product generation.Owing to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C_(2)products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology reconstruction.Thus,this work provides insights into the impact of Nafion on electrocatalytic CO_(2)RR performance.

Calculation of circulation in the South China Sea during summer of 2000 by the modified inverse method

On the basis of hydrographic data obtained in August 2000 cruise, the circulation in the South China Sea (SCS) is computed by the modified inverse method in combination with SSH data from TOPEX/ERS-2 analysis. For study of the dynamical mechanism, which causes the pattern of summer circulation in the SCS, the diagnostic model (Yuan et al. 1982. Acta Oceanologica Sinica,4(1):1-11; Yuan and Su. 1992. Numerical Computation of Physical Oceanography.474-542) is used to simulate numerically the summer circulation in the SCS. The following results have been obtained. (1) The central and southwestern SCSs are dominated mainly by anticy-clonic circulation systems. They are mainly as follows. 1) There is strong anticyclonic eddy southeast of Vietnam (W1). Its horizontal scale is about 300 km, and it extends vertically from the surface to the about 1 000 m level. 2) There are a warm eddy W2 southeast of Zhongsha Islands and the anticyclonic circulation system W3 west off the Luzon Island. 3) There is a stronger cyclonic eddy C1 between the anticyclonic eddies W1 and W2.4) A strong northward coastal jet is present near the coast of Vietnam, and separates from the coast of Vietnam at about 12° N to the northeast.(2)The northern SCS is dominated mainly by a cyclonic circulation system. There is a cyclonic circulation system near and north of Section N2. (3) The southeastern SCS is dominated mainly by the cyclonic circulation system. (4) Comparing the results of circulation in the SCS during the summer of 2000 with those during the summer of 1998, it is found that they agree qualitatively, but there is the some difference between them in quantity.This shows that the circulation in the SCS has obviously seasonal feature. (5) The dynamical mechanism which products the basic pattern of summer circulation is because the following two reasons: 1) the joint effect of the baroclinity and relief (JEBAR) is essential dynamical cause; and 2) it is next important dynamical cause that the interaction between the wind stress and bottom topography under the southerly monsoon. (6) Comparing the hydrographic structure and distribution of stream functions with the SSH data from TOPEX/ERS-2 analysis in the SCS during August of 2000, they agree qualitatively.

Modified (2+1)-dimensional displacement shallow water wave system and its approximate similarity solutions

Recently, a new （2＋1）-dimensional shallow water wave system, the （2＋1）-dlmenslonal displacement shallow water wave system （2DDSWWS）, was constructed by applying the variational principle of the analytic mechanics in the Lagrange coordinates. The disadvantage is that fluid viscidity is not considered in the 2DDSWWS, which is the same as the famous Kadomtsev-Petviashvili equation and Korteweg-de Vries equation. Applying dimensional analysis, we modify the 2DDSWWS and add the term related to the fluid viscidity to the 2DDSWWS. The approximate similarity solutions of the modified 2DDSWWS （M2DDSWWS） is studied and four similarity solutions are obtained. For the perfect fluids, the coefficient of kinematic viscosity is zero, then the M2DDSWWS will degenerate to the 2DDSWWS.

Sensitive Voltammetric Determination of Captopril Using a Carbon Paste Electrode Modified with Nano-TiO_2/Ferrocene Carboxylic Acid

A carbon paste electrode (CPE) modified with ferrocene carboxylic acid (FcCA) and TiO2 nanoparticles was constructed by incorporating TiO2 nanoparticles and ferrocene carboxylic acid into the carbon paste matrix. The electrochemical behavior of captopril (CAP) at the surface of the modified electrode was investigated using electroanalytical methods. The modified electrode showed excellent electrocatalytic activity for the oxidation of CAP in aqueous solutions at physiological pH values. Cyclic voltammetric curves showed that the oxidation of CAP at the surface of the modified electrode reduced its overpotential by more than 290 mV. The modified electrode was used for detecting captopril using cyclic voltammetry and square wave voltammetry techniques. A calibration curve in the range of 0.03 to 2400 μmol/L was obtained that had a detection limit of 0.0096 μmol/L (3?) under the optimized conditions. The modified electrode was successfully used for the determination of captopril in pharmaceutical and biological samples.

Nonlocal symmetry and exact solutions of the(2+1)-dimensional modified Bogoyavlenskii–Schiff equation

In this paper,the truncated Painlev′e analysis,nonlocal symmetry,Bcklund transformation of the（2＋1）-dimensional modified Bogoyavlenskii–Schiff equation are presented.Then the nonlocal symmetry is localized to the corresponding nonlocal group by the prolonged system.In addition,the（2＋1）-dimensional modified Bogoyavlenskii–Schiff is proved consistent Riccati expansion（CRE） solvable.As a result,the soliton–cnoidal wave interaction solutions of the equation are explicitly given,which are difficult to find by other traditional methods.Moreover figures are given out to show the properties of the explicit analytic interaction solutions.

Preparation of the Ag_2O_2-PbO_2 Modified Electrode and Its Application towards Escherichia coli Fast Counting in Water

A novel nano crystalline Ag2O2-PbO2 film chemically modified electrode (CME) was prepared and the CME was characterized by X-ray diffractometer (XRD) and atomic force microscope (AFM). By chronoamperometry, the nano Ag2O2-PbO2 CME was used as bioelectro- chemical sensor to determine the population of Escherichia coli (E. coli) in water. Compared with conventional methods, it is found that the technique we used is fast and convenient in counting E. coli.

Catalytic Oxidation of Dimethyl Ether to Dimethoxymethane over Cs Modified H_3PW_(12)O_(40)/SiO_2 Catalysts

The attractive utilization route for one-step catalytic oxidation of dimethyl ether to dimethoxymethane was successfully carried out over the H3PW12O40（40%）/SiO2 catalyst, modified by Cs, K, Ni, and V. The Cs modification of H3PW12O40（40%）/SiO2 gave the most promising result of 20% dimethyl ether conversion and 34.8% dimethoxymethane selectivity. Dimethoxymethane could be synthe- sized via methoxy groups decomposed from dimethyl ether through the synergistic effect between the acid sites and the redox sites of Cs modified H3PW12O40（40%）/SiO2.

Electrochemical determination of vitamin C in the presence of uric acid by a novel TiO_2 nanoparticles modified carbon paste electrode

The electrochemical behavior of vitamin C（ascorbic acid or AA） is investigated on the surface of a carbon-paste electrode modified with TiO2 nanoparticles and 2,2＇-（1,2 butanediylbis（nitriloethylidyne））-bis-hydroquinone（BBNBH）.The prepared modified electrode showed an efficient catalytic role in the electrochemical oxidation of AA,leading to remarkable decrease in oxidation overpotential and enhancement of the kinetics of the electrode reaction.This modified electrode exhibits well-separated oxidation peaks for AA and uric acid（UA）.The modified electrode is successfully applied for the accurate determination of AA in pharmaceutical preparations.

Synthesis of modified D401 chelating resin and its adsorption properties for Pb^(2+)

A novel chelating resin with sulfonic group was synthesized by chemical modification of D401 resin with sulphonation reaction and characterized by FT-IR spectrometry. The adsorption properties of the novel chelating resin for Pb2+ were studied by batch adsorption, and the adsorption process was analyzed from thermodynamics and kinetics aspects. The adsorption mechanism of Pb2+ on the modified D401 chelating resin was discussed by FT-IR spectrometry. Experimental results show that in the Pb2+ concentration range of 200-400 mg/L, the adsorption capacities of the modified D401 chelating resin for Pb2+ increase by 77%-129%, and Langmuir isothermal adsorption model is more suitable for the equilibrium adsorption data. Adsorption is an endothermic process that runs spontaneously. Kinetic analysis shows that the adsorption rate is mainly governed by liquid film diffusion. The best pH value under adsorption condition is 4-5. The saturated resin can be regenerated by 3 mol/L nitric acid, and the adsorption capacity remains stable after five consecutive adsorption-desorption cycles. The maximal static saturated adsorption capacity of the resin is 206 mg/g at 333 K in the Pb2+ concentration range of 200-400 mg/L. The modified D401 chelating resin is an efficient adsorbent for the removal of Pb2+ from its single-metal ion solution.

Preparation of Calcium Cross-linked Nano-Fe3O4 Modified Zeolite Microspheres for Cu^2+ Adsorption from Wastewater

Artificial zeolite was modified by nano-Fe3O4 for development of functional adsorbents.Subsequently,adsorbents such as calcium cross-linked nano-Fe3O4 microspheres (Ca-MS),calcium cross-linked nano-Fe3O4 modified zeolite microspheres (Ca-MZS) and iron cross-linked nano-Fe3O4 modified zeolite microspheres (Fe-MZS) were prepared and compared for their adsorption performance.The effects of adsorbent dosage,solution pH,initial concentration and ion content on the removal of Cu^2+ from wastewater are investigated,and the adsorption kinetics and isotherms for the adsorbent materials were analyzed.The experimental results indicate that for the initial concentration of Cu^2+ of 30 mg/L,the adsorption is noted to be most stable.The optimal initial pH for adsorbing Cu^2+ is observed to be 5.5.At an optimal dosage of Ca-MZS of 900 mg/L,the adsorption capacity is measured to be 28.25 mg/g,along with the removal rate of 72.49%.The addition of Na+ and K+ affects the adsorption of Cu^2+.For the Na^+ and K^+ concentration of 0.2 mmol/L,the Cu^2+ removal rate by Ca-MZS drops to 11.94% and 22.12%,respectively.As compared with the adsorbents such as Natural Zeolite (NZ),Ca-MS and Fe-MZS,Ca-MZS demonstrates the best removal effect in solution,where the removal rate reaches 84.27%,with the maximum adsorption capacity of 28.09 mg/g.The Cu^2+ adsorption kinetics of Ca-MZS is observed to follow the Elovich kinetic model,with the adsorption isotherm data fitting the Freundlich isotherm model by using the non-linear method.

Formation of TiO2 Modified Film on Carbon Steel

A new technique for preparing TiO2 modified film on carbon steel was accomplished by electroless plating and sol-gel composite process. The artificial neural network was applied to optimize the preparing condition of TiO2 modified film. The optimized condition for forming TiO2 modified film on carbon steel was that NiP plating for 50 min, dip-coating times as 4, heat treatment time for 2 h, and the molar ratio of complexing agent and Ti(OC4HZ9)4 kept 1.5:1. The results showed that TiO2 modified film have good corrosion resistance. The result conformed that it is feasible to design the preparing conditions of TiO2 modified film by artificial neural network.

Satisfactory surgical outcome of T2 gastric cancer after modified D2 lymphadenectomy

Objective： Though D2 lymphadenectomy has been increasingly regarded as standard surgical procedure for advanced gastric cancer （GC）, the modified D2 （D 1＋7, 8a and 9） lymphadenectomy may be more suitable than D2 dissection for T2 stage GC. The purpose of this study is to elucidate whether the surgical outcome of modified D2 lymphadenectomy was comparable to that of standard D2 dissection in T2 stage GC patients. Methods： A retrospective cohort study with 77 cases and 77 controls matched for baseline characteristics was conducted. Patients were categorized into two groups according to the extent of lymphadenectomy： the modified D2 group （roD2） and the standard D2 group （D2）. Surgical outcome and recurrence date were compared between the two groups. Results： The 5-year overall survival （OS） rate was 71.4% for patients accepted mD2 lymphadenectomy and 70.1% for those accepted standard D2, respectively, and the difference was not statistically significant. Multivariate survival analysis revealed that curability, tumor size, TNM stage and postoperative complications were independently prognostic factors for T2 stage GC patients. Patients in the mD2 group tended to have less intraoperative blood loss （P=0.001） and shorter operation time （P〈0.001） than those in the D2 group. While there were no significant differences in recurrence rate and types, especially lymph node recurrence, between the two groups. Conclusions： The surgical outcome of mD2 lymphadenectomy was equal to that of standard D2, and the use of mD2 instead of standard D2 can be a better option for T2 stage GC.

Hot corrosion of modified Ti_3Al-based alloy coated with thin Na_2SO_4 film at 910 and 950℃ in air

The hot corrosion behaviour of a modified Ti3Al-based alloy under thin Na2SO4deposit film was investigated at910and950°C in air.The corrosion product was identified by XRD and its morphologies on the surface and cross-section were observed bySEM.The alloy suffered from considerable hot corrosion attack.The mass gain versus time curves obtained by TGA exhibited tworegions of different kinetics.The whole corroded layer consisted of loose and porous mixture oxides of TiO2,Nb2O5and Al2O3.Numerous small nodules of corrosion product were observed.An illustrative schematic was established to describe the formationprocess of such nodules.It seemed that the refractory oxides played a significantly important role in determining the development ofhot corrosion attack.

Vacancies and Antisites in B2 FeAl and DO_3 Fe_3Al with a Modified Analytic EAM Model

A simple modified analytic EAM model for bcc Fe and fcc Al was used to calculate the lattice constant and elastic constants of B2 FeAl and DO3 Fe3Al alloys. The formation energies of vacancy and antisite were also calculated. The present calculations are in agreement with the experimental data and the theoretical results obtained by other authors.

Improved Stability and Shape Selectivity of 2,6-Dimethylnaphthalene by Methylation of Naphthalene with Methanol on Modified Zeolites

2,6-Dimethylnaphthalene (2,6-DMN) is a key intermediate for polyethylene naphthalate synthesis. The selective synthesis of 2,6-DMN from naphthalene and methanol was carried out over different zeolites (HZSM-5, Hβ, HUSY and SAPO-11) modified by 0.1wt% PdO under atmospheric pressure. Among the adopted zeolites, SAPO-11 exhibits exceptional shape-selectivity and stability to synthesize 2,6-dimethylnaphthalene from methylation of naphthalene, due to the special pore structure of SAPO-11 which inosculated better with 2,6-dimethylnaphthalene than with 2,7-dimethylnaphthalene.

Direct Synthesis of Al_2O_3-modified Li(Ni_(0.5)Co_(0.2)Mn_(0.3))O_2 Cathode Materials for Lithium Ion Batteries

To improve the cyclic stability at high temperature and thermal stability, the spherical Al2O3-modified Li（Ni0.5Co0.2Mn0.3）O2 was synthesized by a modified co-precipitation method, and the physical and electrochemical properties were studied. The TEM images showed that Li（Ni0.5Co0.2Mn0.3）O2 was modified successfully with nano-Al2O3. The discharge capacity retention of Al2O3-modified Li（Ni0.5Co0.2Mn0.3）O2 maintained about 99% after 200 cycles at high temperature（55 ℃）, while that of the bare one was only 86%. Also, unlike bare Li（Ni0.5Co0.2Mn0.3）O2, the Al2O3-modified material cathode exhibited good thermal stability.

Solving (2+1)-dimensional sine-Poisson equation by a modified variable separated ordinary differential equation method

By introducing a more general auxiliary ordinary differential equation （ODE）, a modified variable separated ordinary differential equation method is presented for solving the （2 ＋ 1）-dimensional sine-Poisson equation. As a result, many explicit and exact solutions of the （2 ＋ 1）-dimensional sine-Poisson equation are derived in a simple manner by this technique.

CO_(2) capture by double metal modified CaO-based sorbents from pyrolysis gases

High-temperature pyrolysis technology can effectively solve the problem of municipal solid waste pollution.However,the pyrolysis gas contains a large amount of CO_(2),which would adversely affect the subsequent utilization.To address this problem,a novel method of co-precipitation modification with Ca,Mg and Zr metals was proposed to improve the CO_(2)capture performance.X-ray diffraction(XRD)patterns and energy dispersive X-ray spectroscopy analysis showed that the two inert supports MgO and CaZrO_(3)were uniformly distributed in the modified calcium-based sorbents.In addition,the XRD results indicated that CaZrO_(3)was produced by the reaction of ZrO_(2)and CaO at high temperatures.The effects of doping ratios,adsorption temperature,calcination temperature,CO_(2)concentration and calcination atmosphere on the adsorption capacity and cycle stability of the modified calcium-based sorbent were studied.The modified calcium-based sorbent achieved the best CO_(2)capture performance when the doping ratio was 10:1:1 with carbonation at 700℃ under 20%CO_(2)/80%N_(2)atmosphere and calcination at 900℃ under100%N_(2)atmosphere.After ten cycles,the average carbonation conversion rate of Ca-10 sorbent was 72%.Finally,the modified calcium-based sorbents successfully reduced the CO_(2)concentration of the pyrolysis gas from 37%to 5%.