摘要：Uncovering the structure evolution and real active species of energy catalytic materials under reaction conditions is important for both understanding structure-activity relationship and constructing electrocatalysts for CO2 electroreduction(CO2ER).And integrating CO2ER with an anodic organic transformation to replace the oxygen evolution reaction is highly ***,In2O3 is selected as the model material to reveal the surface reconstruction under CO2ER *** situ and ex situ results reveal that the electrochemical in situ reconstruction of crystalline In2O3 leads to the formation of crystalline-In/amorphous In2O3-x heterostructure(In/In2O3-x).In/In2O3-xacts as the real active phase with Faradaic efficiency of^89.2%for the formate,outperforming In(~67.5%).The improved performance can be ascribed to electron-rich In rectified by Schottky effect of ***,formate and high-value octanenitrile can be simultaneously achieved by integrating CO2ER with octylamine oxidation in an In2O3-x||Ni2P two-electrode electrolyzer.

摘要：有机共晶,由于其光热转换性质,为光热成像、生物应用和海水淡化等诸多领域带来了希望和活力.然而,有机共晶的光热转换机制尤其缺少详细且深入的理论研究.本研究使用含时密度泛函理论方法探索了激发和去激发过程,并解释了DBTTF-TCNB共晶比其组分单晶具有更高光热转换效率的原因.结果显示,高激发态的高占比促进了非辐射跃迁的发生.基于DBTTF-TCNB共晶中给电子基团和吸电子基团间的电荷转移结果,我们发现给体和受体之间吸引电子的竞争可能会促进光热转换,且给电子基团在共晶结构中也十分重要.这些结果可为光热转换共晶的设计提供理论指导.轨道贡献和电子密度差进一步证明了我们的结论.因此,本研究从量子化学的角度给光热共晶在创新领域的应用提供了理论依据.

摘要：The advancement in grazing incidence X-ray scattering(GIWAXS)techniques at synchrotron radiation facilities has significantly deepened our understanding of semiconducting ***,investigation of ultrathin polymer films under tensile conditions poses challenge,primarily due to limitations associated with the lack of suitable sample preparation methods and new stretching *** study addresses these limitations by designing and developing an in-situ temperature-controllable stretching sample stage,which enables real-time structural measurements of ultrathin polymer films at Beijing Synchrotron Radiation *** particular,we report,for the first time,in-situ GIWAXS results of representative semiconducting polymer thin films under variable-temperature *** research has overcome the limitations imposed by sample constraints,thus facilitating the achievement of valuable insights into the behavior of ultrathin polymer films under tensile *** changes in the molecular ordering and packing within the polymer thin films as a result of increasing applied strain and temperature have been *** study promotes future developments in the field,thus enabling the design and optimization of intrinsically stretchable electronic devices and other technologically relevant applications.

摘要：Cocrystal has been discovered and studied for more than 170 years since 1844, while the applications to optoelectronics only begin in the last decade. Several general questions that chemists and materials scientists currently seek to answer are: can we design and control the molecular self-assembly and cocrystal growth, what’s the packing-property correlations, as well as how can we improve device parameters for real applications in industry. In this contribution, we review our and other groups’ recent advances in the cocrystal research field sequentially including:(1) nucleation and growth mechanisms for selective preparation of cocrystals with different donor/acceptor ratio and morphology;(2) charge transport and electronic devices, particularly field-effect transistor(FET) and photo-response device. We discuss the in-situ single crystal device fabrication method, ambipolar charge transport, and molecular packingcharge separation correlation;(3) photonic and optical property, focusing on optical waveguide, photonic logic computation, and nonlinear optics(NLO). We present unusual optical properties revealed by advanced instruments and general structure-function relations for future study. Importantly, the extensive investigations described herein yield in-depth and detailed understandings of molecular cocrystals,and show that such bi-component material systems together with the developed instrument measurement methodologies have the potential to initiate unconventional electronic and photonic science and technology.

摘要：Electrochemical water splitting,as a promising method for hydrogen production,has attracted significant ***,the lack of an electrocatalyst with a small energy loss and fast reaction kinetics has hindered the development of this *** nanomaterials with short-range order and long-range disorder features have recently shown superior activity compared to their crystalline counterparts in water *** enhanced activity arising from their intrinsic disordered structure results in more active sites and a higher intrinsic activity of such *** this regard,this review is aimed at summarizing the progress in amorphous electrocatalysts for water ***,the synthesis strategies for amorphous electrocatalysts are *** tools for amorphous nanomaterials are then ***,the origin of the enhanced activity and stability of amorphous nanomaterials is ***,the current challenges and promising opportunities in this research area are *** review aims to provide a guide for designing and developing amorphous nanomaterials with a fascinating electrocatalytic water splitting performance.

摘要：A room-temperature electrochemical strategy for hydrogenation(deuteration)and reverse dehydrogenation of N-heterocycles over a bifunctional MoNi_(4)electrode is developed,which includes the hydrogenation of quinoxaline using H2O as the hydrogen source with 80%Faradaic efficiency and the reverse dehydrogenation of hydrogen-rich 1,2,3,4-tetrahydroquinoxaline with up to 99%yield and *** in situ generated active hydrogen atom(H^(*))is plausibly involved in the hydrogenation of quinoxaline,where a consecutive hydrogen radical coupled electron transfer pathway is ***,the MoNi_(4)alloy exhibits efficient quinoxaline hydrogenation at an overpotential of only 50 mV,owing to its superior water dissociation ability to provide H^(*)in alkaline *** situ Raman tests indicate that the Ni^(Ⅱ)/Ni^(Ⅲ)redox couple can promote the dehydrogenation process,representing a promising anodic alternative to low-value oxygen ***,electrocatalytic deuteration is easily achieved with up to 99%deuteration ratios using *** method is capable of producing a series of functionalized hydrogenated and deuterated quinoxalines.

摘要：柔性有机突触晶体管(FOSTs)由于其灵活性、生物相容性、易于加工和低复杂性而引起了广泛关注.然而,FOSTs很难在满足装置变形要求的同时保持其突触性质的机械稳定性.在此,我们通过实验发现,弯曲变形对FOSTs的突触性能(即兴奋性突触后电流(EPSC)值)的影响大于对导通电流的影响.此外,通过公式推导,我们证明了通道附近产生的弯曲诱导缺陷状态的密度显著影响突触性能.我们提出了一种使用封装层调整器件稳定段的通用方法.无调节稳定段的普通FOSTs的EPSC值在弯曲后下降了近1.5-2个数量级.相比之下,设计的柔性突触装置表现出相对稳定的EPSC.此外,设计的FOSTs表现出稳定的成对脉冲促进、长期增强和光学突触性能.此外,使用手写人工神经网络在500次弯曲循环前后基于我们的设备进行神经形态计算模拟,该设备在50个学习周期后显示出稳定的识别精度(初始状态下91.55%,500个弯曲周期后90.43%).稳定段在柔性突触晶体管中的成功应用为制造具有机械稳定性的柔性神经形态电子器件提供了一个方便和简单的思路.

摘要：二维分子晶体是一类具有优异光电性能的新兴材料.然而,由于人们对决定二维结晶的因素知之甚少,二维分子晶体的生长极具挑战.我们研究了有机半导体的二维结晶和表面自由能之间的关系,提出了利用表面自由能各向异性因子来衡量二维结晶趋势的设想.以两个BTBT衍生物为例,我们发现具有大的g因子的分子有不受外界条件干扰的二维结晶趋势.这项工作为合理设计可二维结晶的有机半导体提供了指导.

摘要：Advanced oxidation processes(AOPs) have been applied to address multiple environmental concerns including antibiotic resistance genes(ARGs). ARGs have shown an increasing threat to human health,and they are either harbored by antibiotic-resistant bacteria(ARB) or free in the ***, the control of ARGs has been substantially limited by their low concentration and the limited knowledge about their interfacial behavior. Herein, a novel AOP catalyst, Ag/TiO_(2)/graphene oxide(GO),combined with a polyvinylidene fluoride(PVDF) ultrafiltration membrane was designed with a synergistic interfacial adsorption and oxidation function to inactivate ARGs with high efficiency in both model solutions and in secondary wastewater effluent, especially when the residue concentration was *** analysis showed that the mineralization of bases and phosphodiesters mainly caused the inactivation of ARGs. Moreover, the interfacial adsorption and oxidation processes of ARGs were studied at the molecular level. The results showed that GO was rich in sp^(2) backbones and functional oxygen groups,which efficiently captured and enriched the ARGs via p-p interactions and hydrogen bonds. Therefore,the photogenerated active oxygen species attack the ARGs by partially overcoming the kinetic problems in this process. The Ag/Ti O2/GO catalyst was further combined with a PVDF membrane to test its potential in wastewater treatment applications. This work offers an efficient method and a corresponding material for the inactivation and mineralization of intra/extracellular ARGs. Moreover, the molecularlevel understanding of ARG behaviors on a solid–liquid interface will inspire further control strategies of ARGs in the future.

摘要：Photonic synaptic transistors are promising neuromorphic computing systems that are expected to circumvent the intrinsic limitations of von Neumann-based *** design and construction of photonic synaptic transistors with a facile fabrication process and highefficiency information processing ability are highly desired,while it remains a tremendous ***,a new approach based on spin coating of a blend of CsPbBr_(3) perovskite quantum dot(QD)and PDVT-10 conjugated polymer is reported for the fabrication of photonic synaptic *** combination of flat surface,outstanding optical absorption,and remarkable charge transporting performance contributes to high-efficiency photon-to-electron conversion for such perovskite-based ***-performance photonic synaptic transistors are thus fabricated with essential synaptic functionalities,including excitatory postsynaptic current(EPSC),paired-pulse facilitation(PPF),and long-term *** utilizing the photonic potentiation and electrical depression features,perovskite-based photonic synaptic transistors are also explored for neuromorphic computing simulations,showing high pattern recognition accuracy of up to 89.98%,which is one of the best values reported so far for synaptic transistors used in pattern *** work provides an effective and convenient pathway for fabricating perovskite-based neuromorphic systems with high pattern recognition accuracy.