Hybrid Catalyst Coupling Zn Single Atoms and CuNx Clusters for Synergetic Catalytic Reduction of CO2

Reverse water-gas shift (RWGS) reaction is the initial and necessary step of CO₂ hydrogenation to high value-added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnN_x@C-N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four-coordinate Zn-N₄ sites and low valence CuN_x clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn-N₄ and N₄ structures, which show strong Lewis basicity and has strong adsorption for *CO₂ and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO₂ conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO₂ conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu-ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO₂. In the catalytic process, CuN_x not only adsorbs and activates H₂, but also cooperates with the adjacent Zn-N₄ and N₄ structures to jointly activate CO₂ molecules and further promotes the hydrogenation of CO₂. This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts.     

Single-Atom Metal Sites Anchored Hydrogen-Bonded Organic Frameworks for Superior “Two-In-One” Photocatalytic Reaction

Photoredox catalysis is a green solution for organics transformation and CO₂ conversion into valuable fuels, meeting the challenges of sustainable energy and environmental concerns. However, the regulation of single-atomic active sites in organic framework not only influences the photoredox performance, but also limits the understanding of the relationship for photocatalytic selective organic conversion with CO₂ valorization into one reaction system. As a prototype, different single-atomic metal (M) sites (M²⁺ = Fe²⁺, Co²⁺, Ni²⁺, Cu²⁺, and Zn²⁺) in hydrogen-bonded organic frameworks (M-HOF) backbone with bridging structure of metal-nitrogen are constructed by a typical “two-in-one” strategy for superior photocatalytic C N coupling reactions integrated with CO₂ valorization. Remarkably, Zn-HOF achieves 100% conversion of benzylamine oxidative coupling reactions, 91% selectivity of N-benzylidenebenzylamine and CO₂ conversion in one photoredox cycle. From X-ray absorption fine structure analysis and density functional theory calculations, the superior photocatalytic performance is attributed to synergic effect of atomically dispersed metal sites and HOF host, decreasing the reaction energy barriers, enhancing CO₂ adsorption and forming benzylcarbamic acid intermediate to promote the redox recycle. This work not only affords the rational design strategy of single-atom active sites in functional HOF, but also facilitates the fundamental insights upon the mechanism of versatile photoredox coupling reaction systems.     

Flexible and Air-Stable Near-Infrared Sensors Based on Solution-Processed Inorganic–Organic Hybrid Phototransistors

Flexible and air-stable phototransistors are highly demanded for wearable near-infrared (NIR) image sensors. However, advanced NIR sensors via low-cost, solution-based processes remained a challenge. Herein, high-performance inorganic–organic hybrid phototransistors are achieved based on solution processed n-type metal oxide/polymer semiconductor heterostructures of In₂O₃/poly{5,5′-bis[3,5-bis(thienyl)phenyl]-2,2′-bithiophene-3-ethylesterthiophene]} (PTPBT-ET). The In₂O₃/PTPBT-ET hybrid phototransistor combines the advantages of both fast electron transport in In₂O₃ and high photoresponse in PTPBT-ET, showing high saturation mobility of 7.1 cm² V⁻¹ s⁻¹ and large current on/off ratio of >10⁷. As a result, the phototransistor exhibits high performance towards NIR light sensing with a responsivity of 200 A W⁻¹, a specific detectivity of 1.2 × 10¹³ Jones, and fast photoresponse with rise/fall time of 5/120 ms. Remarkably, the hybrid phototransistor, without any passivation, demonstrates excellent electrical stability without performance degradation even after 160 days in air. A 10 × 10 phototransistor array is also enabled by virtue of the high device uniformity. Lastly, flexible In₂O₃/PTPBT-ET phototransistor on polyimide substrate is attained, exhibiting outstanding mechanical flexibility up to 1000 bending/releasing cycles at a bending radius of 5 mm. These achievements pave the way for constructing air-stable hybrid phototransistors for flexible NIR image sensor applications.     

基于等离激元纳米结构非对称集成的二维材料自驱动光响应增强的研究进展（特邀）

金属-二维材料-金属是最常见的二维材料光探测器件的结构。由于结构简单、易于集成,该类器件受到最广泛的关注和研究。其自驱动光探测的模式具有很低的暗电流,有望成为高性能红外探测的新途径。然而金属-二维材料-金属的自驱动光探测存在两个瓶颈问题:（1）反对称的金属-二维材料结区引起的泛光照射下光响应的抵消;（2）二维材料有限光吸收导致的低响应率。文中介绍了利用等离激元纳米结构的非对称集成引入非对称的光耦合,从而打破泛光照射下二维材料与两端电极接触区域产生的光电流的对称性,实现净的自驱动光响应;同时利用等离激元纳米结构产生的局域强光场提高二维材料光吸收率和光响应率的一系列研究进展。在石墨烯等离激元纳米谐振腔复合结构中,实现两个电极附近的光响应对比度超过100倍,突破了对称光耦合导致的光响应抵消的难题。由于具有将入射光耦合成局域模式的优越能力,等离激元纳米谐振腔比亚波长金属光栅更有效地提高石墨烯响应率一个数量级以上。     

小说人物的分布表示及其应用研究

小说是以刻画人物为中心,通过完整的故事情节和具体的环境描写反映社会生活的一种文学体裁。对小说人物进行建模,是小说文本理解和小说文本挖掘的基础性工作。该文构建了大规模的小说语料库,抽取人物及其依存特征,提出基于skip-gram的人物向量训练方法,以人物为目标,以依存特征为上下文,基于训练出的人物向量,探索了小说人物相似度计算、小说人物聚类分析及小说人物画像等应用。实验结果表明,小说人物的分布表示有较好的应用效果。     

复杂背景下全景视频运动小目标检测算法

为解决复杂背景下全景视频中运动小目标检测精度低的问题,提出一种基于复杂背景下全景视频运动小目标检测算法.首先,为降低复杂背景信息的干扰,提高目标检测的精度,采用快速鲁棒性主成分分析(Fast RPCA)算法将全景视频图像的前景背景信息分离,并提取出前景信息作为有效的图像特征;然后,改进更快的基于区域的卷积神经网络(Faster R-CNN)中的区域生成网络(RPN)的候选框尺度大小,使之适应全景图像中的目标尺寸,再对前景特征图进行训练;最后,通过RPN网络和Fast R-CNN网络共享卷积层输出检测模型,实现对全景视频图像中小目标的精准检测.实验结果表明,所提出算法可以有效抑制复杂的背景信息对目标检测精度的影响,并对全景视频图像中的运动小目标具有较高的检测精度.     

硅藻土/纤维素复合助滤剂在微污染原水处理中的应用

以硅藻土和纤维素为原料,通过溶胶-凝胶法制备出了新型硅藻土/纤维素复合助滤剂,探究了各种制备条件对助滤剂的影响,并在高岭土悬浊液中对硅藻土、纤维素和硅藻土/纤维素的助滤性能进行了比较,同时研究了硅藻土/纤维素助滤剂对实际微污染水过滤的影响。研究结果表明:复合助滤剂的最佳制备条件为纤硅比0.67,氨水浓度5.0×10^-4mol/L,蒸馏水/纤维素40 mL/g,EtOH/硅藻土20 mL/g,60℃恒温水浴;硅藻土/纤维素复合助滤剂的助滤性能要明显优于硅藻土和纤维素助滤剂;在微污染原水直接过滤过程中,投加硅藻土/纤维素助滤剂可提高各微污染物的去除率,结合微滤膜深度处理工艺,最终出水水质满足《生活饮用水卫生标准》(GB 5749-2006)的要求。     

传统镶嵌玻璃艺术在当代建筑中的转型与应用

玻璃镶嵌是西方传统的艺术表现形式,其与建筑的成长密切相关,中世纪哥特式建筑的辉煌使镶嵌玻璃艺术达到了前所未有的高度,这种影响力有效的延续至今。进入当代,随着建筑的发展、科技的进步以及观念的更新,镶嵌玻璃艺术创作发生了深刻的变化,镶嵌玻璃突破了传统的束缚,以新颖的形式、前卫的思想、广泛的应用渠道成为经营建筑空间、美化生活环境的重要艺术载体。文章将从传统镶嵌玻璃的起源出发,着眼镶嵌玻璃在当代艺术创作语境中的演变,探寻其转型的根本方式与思维方法,并在建筑中的应用拓展上作出前瞻性的预测。     

城市社区网络民主：内涵、限度与发展路径

网络民主——一种以网络为媒介的新兴民主形式,它的出现给城市社区建设带来了机遇和挑战。杭州市德加社区积极倡导网络民主建设已有多年,通过实证调研并结合城市社区网络民主探讨了内涵,认为网络民主拓宽了居民参与社区管理渠道,营造了平等的＂公共空间＂,创造了全新的网络监督模式,但也存在网络民意缺乏代表性,非理性参与等局限。解决城市社区网络民主发展中存在的这些问题,需要健全的网络道德规范和完善的法律体系,也离不开社区的重视和充足的物质保障,更需采取多种措施调动居民网络参与的积极性。