摘要：Because of its high purity and excellent orientation, mesophase pitch is a superior precursor for high-performance car-bon materials. However, the preparation of top-notch mesophase pitch faces challenges. Catalytic polycondensation at low temperat-ures is more favorable for synthesizing mesophase pitch, because it circumvents the high-temperature free radical reaction of other thermal polycondensation approaches. The reaction is gentle and can be easily controlled. It has the potential to significantly im-prove the yield of mesophase pitch and easily introduce naphthenic characteristics into the molecules, catalytic polycondensation is therefore a preferred method of synthesizing highly spinnable mesophase pitch. This review provides a synopsis of the selective pre-treatment of the raw materials to prepare different mesophase pitches, and explains the reaction mechanism and associated research advances for different catalytic systems in recent years. Finally, how to manufacture high-quality mesophase pitch by using a cata-lyst-promoter system is summarized and proposed, which may provide a theoretical basis for the future design of high-quality pitch molecules.

摘要：p-d轨道之间的相互作用是一种提升电催化性能的有效方法.然而,其对主族金属的电催化CO_(2)还原(eCO_(2)RR)的增强机制尚不清晰.因此,我们向金属Bi纳米片中引入了一系列过渡金属氧化物(TMO:Fe_(2)O_(3)、Co_(3)O_(4)、NiO),并以此研究引入TMO对Bi物种eCO_(2)RR性能的影响.根据原位傅里叶变换红外光谱(FTIR)和CO_(2)-程序升温脱附(TPD)的结果,Bi/TMO中的TMO可以增强CO_(2)的吸附和活化能力.密度泛函理论(DFT)计算结果表明,Bi活性位点^(*)OCHO吸附能及p轨道的优化可以降低CO_(2)到^(*)OCHO过程和^(*)OCHO到HCOOH过程的理论过电位.同时,由于Bi与TMO之间因复合而发生的电子重排也促进了催化剂与反应物之间的电子传输.因此,在热力学和动力学的双重作用下,Bi/TMO中的Bi活性位点表现出最佳的催化能力,在更宽的电位区间内实现了更高的催化活性和甲酸选择性.其中,Bi/Fe_(2)O_(3)的增强效果最为显著.在500 mV的宽电位区间内达到较高的甲酸的法拉第效率(>90%),在-0.8 VRHE时,甲酸的法拉第效率达到最大值99.7%(Bi的1.11倍),甲酸局部电流密度达到12.65 mA cm^(-2)(Bi的1.86倍).这一研究不仅建立了eCO_(2)RR性能增强与引入TMO之间的关系,也为理性设计高性能电催化剂提供了一条实用的、可扩展的途径.

摘要：光生电荷的分离和转移被认为是影响BiVO_(4)基光阳极光电性能的核心因素之一.本文设计了在BiVO_(4)光阳极与析氧助催化剂之间插入空穴提取层的方法.Cu_(2)O作为空穴提取层引入到助催化剂层(FeOOH/NiOOH)和BiVO_(4)之间,可以有效优化空穴的迁移路径,延长光生空穴的寿命,从而提高电极的光电化学性能.与BiVO_(4)相比,调整后的BiVO_(4)/Cu_(2)O/FeOOH/NiOOH光阳极的电荷分离效率从70.6%提高到了92.0%.此外,该光阳极在1.23 VRHE(AM 1.5G照明下)下,还显示出了3.85 mA cm^(-2)的高光电流密度,是BiVO_(4)的2.77倍.我们的研究结果表明,电沉积Cu_(2)O空穴提取层是一种简单且可扩展的方法,能够有效提高BiVO_(4)的光电活性,可用于太阳能驱动水分解领域.

摘要：At present,metal-organic framework(MOF)-derived nano-micro architectures are actively explored for electromagnetic(EM)wave absorption owing to their flexible composition and structural manipulation that enhance dielectric and magnetic ***,the basic design principles in MOF-derived microwave absorption materials have not been *** review is devoted to analyzing design principles in MOF-derived microwave absorption materials from the following perspectives:diverse monomers(ligands and ions of MOFs),topologies,chemical states,and physical *** derived essential information regarding the EM wave absorption mechanism and the structural-functional dependency is also comprehensively ***,a clear insight into the challenges and perspectives of the industrial revolution upgrading in this promising field is proposed.

摘要：CoFe_(2)O_(4)has been widely used for electromagnetic wave absorption owing to its high Snoek limit,high anisotropy,and suitable saturation magnetization;however,its inherent shortcomings,including low dielectric loss,high density,and magnetic agglomeration,limit its application as an ideal *** study investigated a microstructure regulation strategy to mitigate the inherent disadvantages of pristine CoFe_(2)O_(4)synthesized via a sol–gel auto-combustion method.A series of CoFe_(2)O_(4)foams(S0.5,S1.0,and S1.5,corresponding to foams with citric acid(CA)-to-Fe(NO_(3))_(3)·9H_(2)O molar ratios of 0.5,1.0,and 1.5,respectively)with two-dimensional(2D)curved surfaces were obtained through the adjustment of CA-to-Fe^(3+)ratio,and the electromagnetic parameters were adjusted through morphology *** to the appropriate impedance matching and conductance loss provided by moderate complex permittivity,the effective absorption bandwidth(EAB)of S0.5 was as high as 7.3 GHz,exceeding those of most CoFe_(2)O_(4)-based ***,the EAB of S1.5 reached 5.0 GHz(8.9–13.9 GHz),covering most of the X band,owing to the intense polarization provided by lattice defects and the heterogeneous *** three-dimensional(3D)foam structure circumvented the high density and magnetic agglomeration issues of CoFe_(2)O_(4)nanoparticles,and the good conductivity of 2D curved surfaces could effectively elevate the complex permittivity to ameliorate the dielectric loss of pure CoFe_(2)O_(4).This study provides a novel idea for the theoretical design and practical production of lightweight and broadband pure ferrites.

摘要：用于生产高附加值燃料和化学品的电化学CO_(2)还原反应(CO_(2)RR)为实现全球碳中和提供了一种有前景的方法.近年来,单原子催化剂(SACs)由于金属的最大原子利用率和独特的催化性能受到越来越多的关注.相比之下,除了具有单原子催化剂的上述优点外,双原子位点催化剂(DASCs)还可以通过调节另一种相邻金属从而实现更复杂、可调的原子结构.作为SAC的更深层次的延伸,DASCs可以为CO_(2)RR带来新的机遇,最近引起了人们的浓厚兴趣.本文中,我们重点介绍了DASCs在提升CO_(2)RR性能方面的最新进展.首先,根据双原子活性位点的几何结构和电子配置,对DASCs的分类、合成和证实进行了讨论.之后,根据结合型、异核和同核双原子位点对DASCs在CO_(2)RR中的催化应用进行了分类.特别是通过系统地分析反应途径和原子结构,详细总结了DASCs在CO_(2)RR中的构效关系.最后,提出了未来设计DASCs面临的机遇和挑战,以启发设计具有高结构精度和高CO_(2)RR活性、选择性的DASCs.

摘要：光催化氧化有机反应是绿色催化合成转化的重要途径之一.这其中,分子氧活化过程产生活性氧物种(ROS)对促进非均相有机光合成反应选择性具有重要作用,但光催化可控分子氧活化定向生成ROS的研究尚不多见.本研究发现了共轭微孔聚合物(CMPs)的共轭度设计可诱导分子氧活化的选择性.通过CMPs共轭度的设计调控,具有强共轭结构CMP-A材料可促进分子内光生载流子的转移,而弱共轭结构CMP-D材料则会增强光生载流子在其表面的局部积累,使得CMP-A与CMP-D在光催化反应苄胺脱氢偶联与硫醚氧化方面表现出不同性能.研究证实了共轭度诱导的差异化载流子迁移过程可有效促进超氧自由基(·O_(2)^(-))和单线态氧(^(1)O_(2))的定向生成,为理性设计CMPs用以提高多种光催化有机反应的选择性提供新的思路.

摘要：开发高熵硼化物材料的功能特性对于拓宽其在极端环境中的潜在应用至关重要.为此,本文通过调控材料的组分开发出具有高效催化性能的高熵二硼化物(HEB_(2))纳米颗粒:首先基于对HEB_(2)的尺寸差异因子、混合焓以及体系自蔓延燃烧模式的理论分析,我们采用一种简便、快速、低成本的燃烧合成方法合成了6种不同组分的HEB_(2)纳米颗粒;然后,通过对材料的组分进行调控实现了HEB_(2)纳米颗粒活化过硫酸盐降解抗生素的高效催化能力(四环素的最高去除效率可达93.5%).不同吸附位点的吸附能和差分电荷密度的第一性原理计算结果进一步证实了HEB_(2)优异的催化性能主要归因于Ti组元,而非高熵效应.此外,基于检测到的活性氧和计算的反应能垒,我们提出了HEB_(2)活化过硫酸盐降解抗生素的潜在催化机理.本研究不仅为HEB_(2)高效催化降解抗生素的组分设计提供了理论依据,而且显示出HEB_(2)在去除自然水体中新污染物方面的潜在应用前景.

摘要：氧还原反应(ORR)是燃料电池和金属-空气电池等各种能源转换器件中重要的半反应.由于ORR的动力学缓慢,需要开发高活性电催化剂来替代常用的贵金属铂基催化剂.Fe-N-C催化剂被认为是最有前景的材料,其丰富的活性位点可以降低含氧中间体的能垒.在这篇综述中,我们详细总结了Fe-N-C催化剂在理论和实验研究方面的最新研究进展.首先,概述了基于Fe-N-C催化剂的电催化ORR的反应机理.然后,对Fe-N-C催化剂的设计策略和活性位点进行了分类.接下来,讨论了活性位点与催化性能之间的关系.介绍了Fe-N-C催化剂在燃料电池和锌空气电池中的应用现状.最后,进一步提出了Fe-N-C催化剂在可控合成、机理研究和能源器件应用方面面临的挑战和机遇.

摘要：催化效应是实现电极材料高效电化学能量转换和存储的关键因素之一.碳基复合材料因具有优异的物化性能,被广泛地合成并应用于电极材料.电极材料在能源存储器件中表现出的容量往往超过其理论容量值,额外容量的产生原因及形成机制尚未得到准确解释.本文首先回顾了储能器件的研究现状和不足,阐述了催化效应在不同类型能源存储器件中的作用:促进固体电解质界面相的演化,加速放电/充电产物的可逆转化,以及提高中间体的转化速率和活性物质的利用率,从而提升活性物质的利用.此外,还分析了催化效应与储能性能之间的相互作用,以突出催化效应的重要功能.希望本综述在系统地分析、归纳和总结的基础上,为设计具有高效催化作用的电极材料提供新思路,积极推动这一研究领域的发展.