摘要：科学正在进入一个新时代——第五范式——它被认为是知识整合到不同领域的主要特征,是基于无所不在的机器学习系统的计算社区中智能驱动的工作。在此,我们通过在天河一号超级计算机系统上构建的催化材料专门设计的典型平台案例,生动地阐明了第五范式的本质,旨在促进第五范式在其他领域的培养。第五范式平台主要包括模型自动构建(原始数据提取)、指纹自动构建(神经网络特征选择)以及跨学科知识串联的重复迭代(“火山图”)。与分解一起进行的是对迭代中实现的体系结构的性能评估。通过讨论,第五范式的智能驱动平台可以极大地简化和改进研究中极其繁琐和具有挑战性的工作,并通过补偿机器学习中缺少样本和替代一些由于计算资源不足而导致的数值计算来实现数值计算与机器学习之间的相互反馈,从而加速探索过程。在数据驱动的学科中,跨学科专家的协同作用和对动态数据需求的急剧增长仍然是一个挑战。我们相信,对第五范式平台的一瞥可以为其在其他领域的应用铺平道路。

摘要：在电解水制氢过程中,为了在低电位下获得超高电流密度,其关键在于打破氧生成反应的标度关系.本文中,我们设计了一种新型异质界面功能化的NiFe(OH)_(x)/Ni_(3)S_(2)电催化剂,成功地规避了析氧反应(OER)的标度关系,使ΔGHOO*-ΔGHO*的差值从3.20 eV降低到2.38 eV.所制备的NiFe(OH)_(x)/Ni_(3)S_(2)电催化剂仅需要310 mV的过电位即可获得2000 mA cm^(-2)的超高电流密度, Tafel斜率仅为20.8 mV dec^(-1).此外,在1000 mA cm^(-2)的电流密度下,稳定运行100小时后无明显的活性损失,该性能优于目前报道的OER催化剂.进一步利用密度泛函理论计算和实验结果揭示了并联催化作用机制,发现多种中间体吸附能均一化能够优化OER反应路径,从而提升超高电流密度下的OER催化性能.本文的研究结果对开发工业级高性能水分解电催化剂具有重要的指导意义.

摘要：MXene具有丰富的高电负性末端原子、较大的比表面积和较小的原子厚度等优点,已被用作前驱体制备多种纳米材料.然而,目前已报道的用于衍生金属有机框架(MOF)的MXene仅限于V_(2)CT_(x).因此,通过增加MXene和有机配体的种类,合理设计和合成新型MOF,并进一步深入探索其合成机理仍是目前面临的重要挑战.本文采用金属离子辅助转化策略,以二维Ti_(3)C_(2)T_(x)为前驱体,合成了具有非互穿SrSi2(srs)框架的基于儿茶酚的三维(3D)TiCu-HHTP(HHTP=2,3,6,7,10,11-六羟基三苯)MOF.该策略表现出了良好的普适性,Ti3C2和辅助Cu^(2+)离子可以扩展到V2C MXene和其他辅助金属离子Mn^(+)(M=Ni^(2+)、Co^(2+),Mn^(2+)和Zn^(2+)).转化机制包括从Ti3C2纳米片到辅助金属离子的电荷转移、Ti-C键断裂促进释放Ti^(4+)离子以及Ti^(4+)/Mn^(+)与HHTP之间的强螯合配位协同促进TiCu-HHTP的形成.独特的3D导电网络和丰富的氧化还原位点赋予了TiCu-HHTP-7/PPy复合柔性透明电极快速的离子/电子传输和可逆的法拉第反应.在0.02 mA cm^(-2)电流密度下,TiCu-HHTP/PPy透明电极的面积比电容值达到3.63 mF cm^(-2),明显高于纯PPy电极的面积电容值(1.79 mF cm^(-2)).TiCu-HHTP/PPy透明电容器在0.75μW cm^(-2)的功率密度下,能量密度为0.042μWh cm^(-2).

摘要：开发钙钛矿叠层太阳电池是一种可以突破单结太阳电池Shockley-Queisser极限的光伏技术.令人鼓舞的是,所有钙钛矿叠层器件,包括钙钛矿/硅、钙钛矿/钙钛矿、钙钛矿/铜铟镓硒和钙钛矿/有机叠层电池,都表现出比相应单结太阳电池更高的效率,显示出巨大的进一步突破的潜力.在叠层器件中,电荷传输材料是钙钛矿子电池的重要组成部分,它直接决定了器件的电荷传输和能量损失.一般来说,高导电性和透光性、良好的能级和化学稳定性是电荷传输材料叠层应用的关键.迄今为止,导电金属氧化物、有机分子、聚合物、富勒烯、自组装材料等各种电荷传输材料已被广泛应用于高效叠层电池.在本文中,我们首先总结了不同类型钙钛矿叠层电池的电荷传输材料的最新进展,详细讨论了材料的电学和光学性质及其对器件性能的影响.在此基础上,我们提出了叠层电池中电荷传输材料进一步发展所面临的挑战和展望.本综述将为不同钙钛矿叠层太阳电池的器件设计提供有效指导.

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：钾离子电池(PIBs)面临的一个关键问题是设计具有先进结构的负极材料,以实现快速电荷传输以提高钾的存储性能.采用碳二亚胺铁(FeNCN)作为阳极,由于其含有一定数量的共价键且在分子水平上具有稳定的结构,使得储钾系统能够实现优异的电化学性能.FeNCN阳极具有高导电性,带隙接近0 eV,并且由于其共价键结构具有良好的结构稳定性.此外,无定形反应产物也为离子扩散提供了多种途径.因此,FeNCN阳极表现出高可逆比容量(在50 mA g^(-1)电流密度下具有600 mA h g^(-1)比容量),显著的倍率性能和长寿命循环(电流密度为500 mA g^(-1)时拥有400 mA h g^(-1)比容量且超过300次循环).通过理论模拟、X射线原位衍射分析和X射线光电子能谱分析揭示了Fe^(2+)和K^(+)之间的转化反应机理.此外,将FeNCN负极与苝-3,4,9,10-四羧酸二酐正极材料匹配,组装成的全电池在198.6 Wkg^(-1)的功率密度下实现了184.7 W h kg^(-1)的超高能量密度,明显高于以往所有铁基负极的PIBs或钾离子混合电容器.

摘要：Binuclear ruthenium complexes bearing the2,2'‐bipyridine‐6,6'‐dicarboxylate(bda)ligand have been demonstrated to be highly active catalysts towards water oxidation with CeIV as an ***,the catalytic properties of ruthenium dimers have not yet been explored for visible light‐driven water ***,the photocatalytic performance of a dipyridyl propane‐bridged ruthenium dimer2was investigated in comparison with its monomeric precursor,[Ru(bda)(pic)2](1),in CH3CN/phosphate buffer mixed solvent in a three‐component system including a photosensitizer and a sacrificial electron *** results showed that the activity of each catalyst was strongly dependent on the content of CH3CN in the phosphate buffer,which not only affected the driving force for water oxidation,but also altered the kinetics of the reaction,probably through different mechanisms associated with the O–O bond *** a result,dimer2showedsignificantly higher activity than monomer1in the solvent containing a low content of CH3CN,and comparable activities were attained with a high content of CH3CN in the *** the optimal conditions,complex2achieved a turnover number of638for photocatalytic O2evolution.

摘要：The selective catalytic hydrogenation of carboxylic acids is an important process for alcohol production,while efficient heterogeneous catalyst systems are still being ***,we report the selective hydrogenation of carboxylic acids using earth‐abundant cobalt oxides through a reaction‐controlled catalysis *** further reaction of the alcohols is completely hindered by the presence of carboxylic acids in the reaction *** partial reduction of cobalt oxides by hydrogen at designated temperatures can dramatically enhance the catalytic activity of pristine samples.A wide range of carboxylic acids with a variety of functional groups can be converted to the corresponding alcohols at a yield level applicable to large‐scale *** monoxide was established as the preferred active phase for the selective hydrogenation of carboxylic acids.

摘要：电化学CO_(2)还原(CO_(2)RR)是一种很有前景的技术,可以将二氧化碳转化为多种增值化学品,从而达到减缓温室效应的目的.然而,实现目标产品的高催化活性、选择性和稳定性仍然是一个很大的挑战.本文通过还原Sn掺杂的Bi2S3制备了间隙掺杂的Snx-Bi (x为Sn与Bi的原子比,x=1/2,1/16,1/24或1/40)纳米线束(NBs).值得注意的是,Sn1/24-Bi NBs在1400 mV的宽电位窗口内表现出超高的甲酸盐选择性(从-0.5到-1.9 V vs.可逆氢电极(RHE),法拉第效率超过90%),在-1.9 V ***时,电流密度达到了-319 mA cm^(-2),可满足工业使用需求.此外,还实现了在~-200 mA cm^(-2)条件下超过84 h的超长稳定性.实验结果和密度泛函理论计算表明,间隙掺杂Sn优化了*OCHO中间体的吸附亲和力,降低了铋催化剂的电子转移能垒,从而获得了显著的CO_(2)RR性能.本研究为设计具有优异催化活性、选择性和耐久性的掺杂型电催化剂用于CO_(2)RR为甲酸盐提供了启示.

摘要：Tissue implant-related infections are among the most serious complications after surgical implantation,including orthopedics and *** with antibacterial ion release systems are efficient and economical antibiotic substitutes to fight against bacterial ***,the excessive amount of released antibacterial ions may cause biological toxicity while killing *** raises a fundamental issue on how to properly control the amounts of ions and their ***,we develop low-dose antibacterial ions-incorporated ferroelectric implants(copper-doped potassium sodium niobate,K0.5Na0.5NbO3-Cu,KNNCu)whose surface potential can be tuned via external *** released Cu2+ions can be targeted to bacteria via endogenous electric field(EEF)between KNNCu implants and negatively charged ***,the antibacterial efficacy of the implants is determined by the amount of Cu^2+ions that reaches bacteria,instead of the total amount of released Cu2+*** amount of Cu2+ions reaching bacteria from the high-surface-potential implant is 2.4 times that from the lowsurface-potential implant within 12 h,resulting in the increased antibacterial ratio from about 65%to 100%,while remaining low cell *** work provides insights into the specific role of the EEF in guiding mass transport between charged materials and living organisms,and a new perspective for the design of high-performance antibacterial biomaterials.