Optimizing the quasi-equilibrium state of hot carriers in all-inorganic lead halide perovskite nanocrystals through Mn doping: fundamental dynamics and device perspectives

Hot carrier (HC) cooling accounts for the significant energy loss in lead halide perovskite (LHP) solar cells. Here, we study HC relaxation dynamics in Mn-doped LHP CsPbI₃ nanocrystals (NCs), combining transient absorption spectroscopy and density functional theory (DFT) calculations. We demonstrate that Mn²⁺ doping (1) enlarges the longitudinal optical (LO)–acoustic phonon bandgap, (2) enhances the electron–LO phonon coupling strength, and (3) adds HC relaxation pathways via Mn orbitals within the bands. The spectroscopic study shows that the HC cooling process is decelerated after doping under band-edge excitation due to the dominant phonon bandgap enlargement. When the excitation photon energy is larger than the optical bandgap and the Mn²⁺ transition gap, the doping accelerates the cooling rate owing to the dominant effect of enhanced carrier–phonon coupling and relaxation pathways. We demonstrate that such a phenomenon is optimal for the application of hot carrier solar cells. The enhanced electron–LO phonon coupling and accelerated cooling of high-temperature hot carriers efficiently establish a high-temperature thermal quasi-equilibrium where the excessive energy of the hot carriers is transferred to heat the cold carriers. On the other hand, the enlarged phononic band-gap prevents further cooling of such a quasi-equilibrium, which facilitates the energy conversion process. Our results manifest a straightforward methodology to optimize the HC dynamics for hot carrier solar cells by element doping.

Mn doping modulates the hot carrier dynamics in all-inorganic lead halide perovskite nanocrystals according to the excitation energy.     

反胶束法制备直接甲醇燃料电池Pt-Sn/C催化剂及其表征

在水/AOT/环己烷反胶束体系中, 制备了Pt-Sn/C催化剂, 研究了不同ω (反胶束溶液中水与表面活性剂的物质量之比)值对Pt-Sn粒径的影响. 并采用TEM, XRD, XPS, 循环伏安等技术对其进行表征. TEM结果表明合成的Pt-Sn纳米颗粒为球形, 在碳载体表面均匀分布, 粒径分布窄, 平均粒径为2.7 nm. Pt-Sn颗粒尺寸随着ω的增加而增大. XRD结果表明该催化剂中Pt具有面心立方结构且没有与Sn形成合金. XPS结果表明在该催化剂中, Pt主要以零价态存在. 在甲醇溶液中的循环伏安扫描结果表明, 甲醇氧化峰电位和峰电流随着ω的增加而减小, 说明反胶束方法可以通过控制颗粒尺寸, 从而影响催化剂的电氧化活性. 相对于商用Pt-Ru/Vulcan XC-72 (20 wt%, E-TEK公司), 该催化剂具有较低的峰电势以及较高的I_f/I_b (循环伏安曲线中正向扫描峰电流与反向扫描峰电流的比值), 这表明用此方法制备的Pt-Sn/C催化剂具有较好的抗中毒能力.     

反应条件对钌基氨合成催化剂性能的影响

用氨合成催化剂性能评价装置,研究了反应温度、压力、空速和氢氮比对以活性炭为载体的钌基氨合成催化剂活性的影响。研究表明,低于400℃时,随着反应温度降低,催化剂的活性急剧降低。随着压力升高,催化剂活性增大。但钌催化剂具有较高的低压活性,适宜低压合成氨。随着空速的降低,催化剂的活性明显提高。在空速和压力一定的条件下,最佳氢氮比随反应温度而异,并且当空速较高或反应温度较低时,氢氮比的变化对催化剂活性的影响更加明显。     

微波作用下卤素交换氟化制备氟代苯甲醛及二苯甲酮类化合物

在微波作用下,采用高效催化剂体系,于中等极性非质子溶剂中经卤素交换氟化高效制备了系列含氟芳香醛(酮)类化合物,产品收率53·3%~92·6%,反应时间较常规加热最多可缩短80%以上。采用中等极性反应溶剂,还可突出表现出微波对反应促进的“非热效应”,从而大大拓宽了氟化反应溶剂的选择范围。     

Plasma assisted synthesis of LiNi0.6Co0.2Mn0.2O2 cathode materials with good cyclic stability at subzero temperatures

Layered Ni-rich cathode materials,LiNi_0.6Co_0.2Mn_0.2O₂(NCM622),are synthesized via solid reaction assisted with a plasma milling pretreatment,which is resulted in lowering sintering temperatures for solid precursors.The plasma milling pretreated NCM622 cathode material sintered at 780℃(named as PM-780)demonstrates good cycling stability at both room and subzero temperatures.Specifically,the PM-780 cathode delivers an initial discharge capacity of 171.2 mAh g^-1 and a high capacity retention of 99.7%after 300 cycles with current rate of 90 mA g^-1 at 30℃,while stable capacities of 120.3 and 94.0 m Ah g^-1 can be remained at-10℃and-20℃in propylene carbonate contained electrolyte,respectively.In-situ XRD together with XPS and SEM reveal that the NCM622 cycled at-10℃presented better structural stability and more intact interface than that of cathodes cycled at 30℃.It is also found that subzero temperatures only limit the discharge potential of NCM622 without destroying its structure during cycling since it still exhibits high discharge capacity at 30℃after cycled at subzero temperatures.This work may expand the knowledge about the low-temperature characteristics of layered cathode materials for Li-ion batteries and lay the foundation for its further applications.     

Cr掺杂对Nd0.7Sr0.3MnO3电磁性质的影响

我们对多晶样品Nd0.7Sr0.3Mn1-xCrxO3(x≤0.30)进行了X射线衍射谱、电阻温度关系和磁化强度测量.实验发现:随Cr掺杂量的增加,样品的电阻率变大,电阻峰温度和居里温度降低,这是由Cr的介入弱化了双交换作用所致;在x=0.10附近,电阻出现了双峰现象,在其M~T上没有发现与低温峰对应的磁性异常;在锰位磁矩与Cr含量的关系中发现,Cr掺杂对样品的磁性几乎无贡献;通过分析,我们用相分离的图象解释了有关的现象.     

基于小波包分析的心磁信号消噪

心磁图(Magnetocardiography)是一种无创性记录和分析心脏电磁场的方法.由于心磁场强度极其弱小,必须使用超导量子干涉仪(SQUID)才能检测,其中心磁信号消噪处理十分重要.本文对心磁测量中的消噪进行了研究,在小波分析的基础上,提出使用小波包分析方法消噪,通过实验发现小波包分析消噪能获得很好的效果.     

Comparative Phosphoproteomic Analysis of Sporulated Oocysts and Tachyzoites of Toxoplasma gondii Reveals Stage-Specific Patterns

Toxoplasma gondii is an obligate intracellular protozoan of severe threat to humans and livestock, whose life history harbors both gamic and apogamic stages. Chinese 1 (ToxoDB#9) was a preponderant genotype epidemic in food-derived animals and humans in China, with a different pathogenesis from the strains from the other nations of the world. Posttranslational modifications (PTMs) of proteins were critical mediators of the biology, developmental transforms, and pathogenesis of protozoan parasites. The phosphoprotein profiling and the difference between the developmental phases of T. gondii, contributing to development and infectivity, remain unknown. A quantitative phosphoproteomic approach using IBT integrated with TiO₂ affinity chromatography was applied to identify and analyze the difference in the phosphoproteomes between the sporulated oocysts and the tachyzoites of the virulent ToxoDB#9 (PYS) strain of T. gondii. A total of 4058 differential phosphopeptides, consisting of 2597 upregulated and 1461 downregulated phosphopeptides, were characterized between sporulated the oocysts and tachyzoites. Twenty-one motifs extracted from the upregulated phosphopeptides contained 19 serine motifs and 2 threonine motifs (GxxTP and TP), whereas 16 motifs identified from downregulated phosphopeptides included 13 serine motifs and 3 threonine motifs (KxxT, RxxT, and TP). Beyond the traditional kinases, some infrequent classes of kinases, including Ab1, EGFR, INSR, Jak, Src and Syk, were found to be corresponding to motifs from the upregulated and downregulated phosphopeptides. Remarkable functional properties of the differentially expressed phosphoproteins were discovered by GO analysis, KEGG pathway analysis, and STRING analysis. S8GFS8 (DNMT1-RFD domain-containing protein) and S8F5G5 (Histone kinase SNF1) were the two most connected peptides in the kinase-associated network. Out of these, phosphorylated modifications in histone kinase SNF1 have functioned in mitosis and interphase of T. gondii, as well as in the regulation of gene expression relevant to differentiation. Our study discovered a remarkable difference in the abundance of phosphopeptides between the sporulated oocysts and tachyzoites of the virulent ToxoDB#9 (PYS) strain of T. gondii, which may provide a new resource for understanding stage-specific differences in PTMs and may enhance the illustration of the regulatory mechanisms contributing to the development and infectivity of T. gondii.     

p-Adic函数空间上Hardy型算子的多线性交换子估计

在p-adic域上研究分数次Hardy型算子与CMO(Qnp)函数生成的多线性交换子,建立了交换子在Lebesgue空间和Herz空间上的有界性.对Hardy算子的多线性交换子也得到了相应的结果.