利用空间位阻和氢溢流协同作用促进5-羟甲基糠醛选择性加氢制备5-甲基糠醛

Selective hydrogenation is a vital class of reaction. Various unsaturated functional groups in organic compounds, such as aromatic rings, alkynyl (C≡C), carbonyl (C＝O), nitro (-NO₂), and alkenyl (C＝C) groups, are typical targets in selective hydrogenation. Therefore, selectivity is a key indicator of the efficiency of a designed hydrogenation reaction. 5-(Hydroxymethyl)furfural (HMF) is an important platform compound in the context of biomass conversion, and recently, the hydrogenation of HMF to produce fuels and other valuable chemicals has received significant attention. Controlling the selectivity of HMF hydrogenation is paramount because of the different reducible functional groups (C＝O, C-OH, and C＝C) in HMF. Moreover, the exploration of new routes for hydrogenating HMF to valuable chemicals is becoming attractive. 5-Methylfurfural (MF) is also an important organic compound; thus, the selective hydrogenation of HMF to MF is an essential synthetic route. However, this reaction has challenging thermodynamic and kinetic aspects, making it difficult to realize. Herein, we propose a strategy to design a highly efficient catalytic system for selective hydrogenation by exploiting the synergy between steric hindrance and hydrogen spillover. The design and preparation of the Pt@PVP/Nb₂O₅ catalyst (PVP = polyvinyl pyrrolidone; Nb₂O₅ = niobium(V) oxide) were also conducted. Surprisingly, HMF could be converted to MF with 92% selectivity at 100% HMF conversion. The reaction pathway was revealed through the combination of control experiments and density functional theory calculations. Although PVP blocked HMF from accessing the surface of Pt, hydrogen (H₂) could be activated on the surface of Pt due to its small molecular size, and the activated H₂ could migrate to the surface of Nb₂O₅ through a phenomenon called H₂ spillover. The Lewis acidic surface of Nb₂O₅ could not adsorb the C＝O group but could adsorb and activate the C-OH group of HMF; therefore, when HMF was adsorbed on Nb₂O₅, the C-OH groups were hydrogenated by the spilled over H₂ to form MF. The high selectivity of this reaction was realized because of the unique combination of steric effects, hydrogen spillover, and tuning of the electronic states of the Pt and Nb₂O₅ surfaces. This new route for producing MF has great potential for practical application owing to its discovered advantages. We believe that this novel strategy can be used to design catalysts for other selective hydrogenation reactions. Furthermore, this study demonstrates a significant breakthrough in selective hydrogenation, which will be of interest to researchers working on the utilization of biomass, organic synthesis, catalysis, and other related fields.      

Lorentz-Minkowski空间中旋转W超曲面

1841年,D elaunay获得如下定理:如果在一平面上沿定直线滚动一条二次圆锥直线,然后将其焦点的轨迹绕定直线旋转,则所得到的曲面具有常数平均曲率,反之,所有旋转常数平均曲率曲面(除球面外)都有如此构造.本文将以上的D elaunay定理推广到Lorentz-M inkow sk i空间Rn1 1中类空的Sm型旋转W超曲面.     

含有五个反馈权值的二维细胞神经网络可实现Mosaic模式

研究一类含有五个反馈权值二维细胞神经网络系统,以系统的输出反馈权值及阈值为参数构成参数空间,引入几何方法,将此空间分解分块成有限个区域,当输出反馈权值及阈值在某一区域上时,给出系统具有M osaic解所有可能的输出函数M osaic模式的充要条件.     

加拿大推出能即时监测空气质量的可穿戴设备

<正>加拿大一新创公司推出了一款新型可穿戴设备,称为TZOA包围追踪器,可以即时监测人们周围的环境状况,如空气质量、紫外线强度等。据物理学家组织网不久前报道,在设计上,这种配置器可以直接检测环境中的空气污染和紫外线强度,TZOA通过蓝牙向智能手机发送并共享数据,i OS和安卓的App(应用程序)就会显示环境指标,指示空气污染和紫外线对用户     

二种求算晶体平面间距d_(hkl)的数学方法

用数学方法推导出结构化学晶体学中晶面间距的一般通式,并在此基础上推导出其他晶系的晶面间距(d(hkl))的计算表达式。     

基于小目标类别注意力机制与特征融合的AF-ICNet非结构化场景语义分割方法

针对非结构化道路分割难度大、小目标检测精度较低等问题,构建基于小目标类别注意力机制与特征融合的AF-ICNet轻量级实时语义分割网络。采用空洞空间卷积池化金字塔融合不同尺度特征感受野以增强网络的全局感知能力。嵌入CA注意力机制,建立通道信息和空间位置信息以增强网络对非结构化道路小目标类别语义特征的提取能力。针对类别分布不均衡问题,改进权重交叉熵损失函数。利用AF-ICNet模型对Cityscapes与IDD数据集进行训练,在Cityscapes测试图像中分割的MIoU达到了71.5%,在IDD测试图像中分割的MIoU达到了62.5%。搭建实验测试系统进行实景测试,测试结果表明,AF-ICNet有效提升了非结构化道路及小目标类别的分割精度,并满足测试的实时性要求。     

空间走离对量子光学频率梳压缩特性的影响

量子光学频率梳在量子计算、量子信息以及高精度量子测量等领域都有重要的价值,同步泵浦光学参量振荡器是制备量子光频梳最主要的手段.本文采用中心波长为815 nm、脉冲宽度为130 fs的锁模飞秒脉冲激光二次谐波泵浦Ⅰ类共线BiB₃O₆晶体以制备真空压缩态量子光频梳,给出了同步泵浦光学参量振荡器中空间走离效应对获得量子光频梳压缩度的影响.研究表明,随着晶体长度的增加,压缩度的增长会受到空间走离效应限制,经计算在晶体长度为1.49 mm时压缩达到最大.在此基础上,本文实验研究了在四种晶体长度下获得的真空压缩态量子光频梳的压缩特性,当BiB₃O₆长度为1.5 mm时获得了(3.6±0.2) dB的最大真空压缩,考虑损耗后为(7.0±0.2) dB,实验结果与理论分析相符.该研究揭示了飞秒脉冲光在非线性晶体中存在的空间走离效应是影响量子光频梳压缩特性的重要因素,为优化量子光频梳的实验测量提供了指导.     

基于1,2-二氰基苯/聚合物复合材料的高耐久性有机阻变存储器

本文报道了一种基于1,2-二氰基苯(O-DCB)与聚(3-己基噻吩)(P3HT)复合薄膜的高耐久性有机阻变存储器(ORSM).ORSM表现出非易失型和双极性存储特性,电流开关比(I_on/off)超过10⁴,耐久性高达400次,保持时间为10⁵s,V_set和V_reset分别为-6.9 V和2.6 V.器件的阻变机理是陷阱电荷的俘获与去俘获,即负偏压或正偏压诱导电荷陷阱的填充和抽离过程,导致电荷传输方式的改变,从而产生高低电阻间的切换.器件的高耐久性一方面是由于O-DCB较小的分子尺寸和较好的溶解性形成了均匀分布且稳定的电荷陷阱,另一方面是由于O-DCB较好的分子平面促进了其与P3HT共轭链的相互作用.该研究为高耐久性ORSM的实现提供了一种有效途径,加快了ORSM的商业化应用进程.     

高中化学竞赛中电子效应和空间效应考点分析——以近年全国化学奥林匹克竞赛试题为例

电子效应和空间效应是有机化学的基础,近年来,这部分知识在全国化学奥林匹克竞赛中的考查比例处于上升趋势。因此,以近年全国化学奥林匹克竞赛试题为例,详细说明电子效应和空间效应在竞赛中的考点,帮助辅导化学竞赛的教师和参加化学竞赛的考生了解该部分知识需要达到的教学标准和掌握层次。     

单细胞与空间转录组分析研究进展

单细胞的异质性在胚胎发育、神经系统发育、癌症病变等生物学过程中具有重要的研究意义。单细胞转录组测序利用测序技术解析细胞内转录本序列,为细胞异质性研究提供可靠、准确的研究手段及观测视野,为揭示生物发育规律、疾病发生发展机制等提供了重要的技术手段。该文围绕单细胞与空间组学分析,综述了近年来发展的各类单细胞转录组测序、单细胞多组学测序及空间转录组分析方法,分析了其优缺点。同时展望了单细胞与空间转录组分析领域的发展趋势,即开发低成本、全方位、高通量、高分辨的单细胞空间多组学分析方法以实现对单个细胞更为细致、全面及准确的描述和精准单细胞图谱构建。