A Generalized Surface Chalcogenation Strategy for Boosting the Electrochemical N2 Fixation of Metal Nanocrystals

Electrocatalytic nitrogen reduction reaction (NRR) is a promising process relative to energy-intensive Haber–Bosch process. While conventional electrocatalysts underperform with sluggish paths, achieving dissociation of N₂ brings the key challenge for enhancing NRR. This study proposes an effective surface chalcogenation strategy to improve the NRR performance of pristine metal nanocrystals (NCs). Surprisingly, the NH₃ yield and Faraday efficiency (FE) (175.6 ± 23.6 mg h^–1 g^–1_Rh and 13.3 ± 0.4%) of Rh-Se NCs is significantly enhanced by 16 and 15 times, respectively. Detailed investigations show that the superior activity and high FE are attributed to the effect of surface chalcogenation, which not only can decrease the apparent activation energy, but also inhibit the occurrence of the hydrogen evolution reaction (HER) process. Theoretical calculations reveal that the strong interface strain effect within core@shell system induces a critical redox inversion, resulting in a rather low valence state of Rh and Se surface sites. Such strong correlation indicates an efficient electron-transfer minimizing NRR barrier. Significantly, the surface chalcogenation strategy is general, which can extend to create other NRR metal electrocatalysts with enhanced performance. This strategy open a new avenue for future NH₃ production for breakthrough in the bottleneck of NRR.     

A Polyallylamine Anchored Amine‐Rich Laser‐Ablated Graphene Platform for Facile and Highly Selective Electrochemical IgG Biomarker Detection

Current immunosensors have an insufficient number of binding sites for the recognition of biomolecules, which leads to false positive or negative results. In this research, a facile, cost‐effective, disposable, and highly selective electrochemical immunosensing platform is developed based on cationic polyelectrolyte polyallylamine (PAAMI) anchored laser‐ablated graphene (LAG). Here, for the first time, PAAMI is introduced to stabilize LAG flakes, while retaining the intrinsic thermal and electronic properties of the substrate by noncovalent π–π interaction and electrostatic physical absorption. The sensing platform offers a suitable number of anchoring sites for the immobilized antibodies by providing ? NH₂ functional groups. The proper grafting of PAAMI is confirmed through X‐ray photoelectron spectroscopy and Raman spectroscopy. The immunosensing platform is applied to detect immunoglobulin (IgG) biomarkers as a proof of concept. Under optimized conditions, the sensing platform exhibits a linear range of 0.012–15 and 15–352 ng mL^?1 with a limit of detection of 6 pg mL^?1 for IgG detection with high selectivity. Based on the analysis, the developed immunosensing platform can be used for point‐of‐care detection of IgG in clinical diagnostic centers. Furthermore, the developed strategy is well suited for the detection of other cancer biomarkers after immobilizing the relevant antibodies.     

回弹检测法检测混凝土强度相关问题的探讨

本文就当前社会人们对建筑安全水平和质量要求不断提高的背景下,对回弹检测法检测混凝土强度的相关问题进行探讨,并以此推动回弹法检测混凝土强度行业标准的规范化发展进程,希望能够给从事相关行业的工作者提供帮助。     

Window Detection in Facades Using Heatmap Fusion

Journal of Computer Science and Technology - Window detection is a key component in many graphics and vision applications related to 3D city modeling and scene visualization. We present a novel...     

污泥生物炭中氮硫行为及环境效应研究进展

污泥生物炭中氮硫元素含量高，其氮硫行为和环境效应对全球气候变化的影响不容忽视。以往的研究中，研究者往往以富碳生物炭作为主要研究对象，关注碳对全球气候变化的行为和功效，而对氮硫元素的作用关注不够。本文从原始污泥基本性质到其热解过程，再到生物炭的老化，逐步对污泥生物炭整个生命周期内氮硫的行为及其环境效应研究进行综述，并对未来应注重开展的研究方向进行展望，为生物炭中氮硫元素固定、释放及与之关联的环境效应和温室气体排放控制研究提供理论基础。分析表明，污泥中氮元素含量普遍高于硫元素，且热解过程中氮比硫更容易转移至气相产物。氮硫元素随热解温度的增加，在三相产物中的分配都是炭中持续减少，油中先增后减，气中一直增加。高温（＞800℃）条件下，气相中的氮含量高于固相，而硫元素则仍然主要存在于固相中。污泥生物炭老化及其环境效应研究表明，污泥生物炭氮硫元素与土壤的相互作用及其温室效应问题在今后的研究中应引起重视。     

宽带毫米波大规模MIMO系统中低复杂度波束域信道估计

针对宽带毫米波大规模MIMO系统信道估计精度低及实现复杂度较高的问题，在传统支撑检测方案的基础上提出一种基于Gauss-Seidel方法的串行支撑检测（GS-SSD）方案。该方案不使用共同支撑假设，参考串行干扰删除，将整体信道估计问题分解为一系列子问题，每个子问题仅考虑一个信道成分。同时，利用Gauss-Seidel方法近似高复杂度的矩阵求逆。仿真结果表明，相比于基于串行支撑检测（SSD）的方案， GS-SSD方案在将求逆复乘数降低一个数量级的同时可以取得接近SSD方案的信道估计性能。     

不同含量低污染水对人工湿地中细菌的影响研究

探究水平流人工湿地(HFCW)系统处理低污染水过程中,相同COD/ρ(TN)下不同碳氮含量对细菌群落结构的影响。结果表明,进水为较高碳氮含量的HFCW(HF1)和进水为较低碳氮含量的HFCW(HF2)对COD和TN的去除效率具有一定的差异,HF1和HF2对COD的去除效率分别为48.26%和28.89%,对TN的去除率分别为79.06%和81.87%。HF1中细菌的丰富度和多样性均高于HF2,HF1中富集的优势细菌为Chloroflexaceae、Comamonadaceae和Rhodocyclaceae,均具有异养反硝化功能,HF2中富集的优势细菌为Xanthomonadaceae和Rhodocyclaceae,其中Xanthomonadaceae具有自养反硝化功能。COD、NH4^+-N和NO3^--N对HF1中细菌群落的影响大于对HF2中细菌群落的影响,HF1中COD对细菌群落的影响大于NH4^+-N和NO3^--N。     

Photoactive Earth‐Abundant Iron Pyrite Catalysts for Electrocatalytic Nitrogen Reduction Reaction

The generation of ammonia, hydrogen production, and nitrogen purification are considered as energy intensive processes accompanied with large amounts of CO₂ emission. An electrochemical method assisted by photoenergy is widely utilized for the chemical energy conversion. In this work, earth‐abundant iron pyrite (FeS₂) nanocrystals grown on carbon fiber paper (FeS₂/CFP) are found to be an electrochemical and photoactive catalyst for nitrogen reduction reaction under ambient temperature and pressure. The electrochemical results reveal that FeS₂/CFP achieves a high Faradaic efficiency (FE) of ≈14.14% and NH₃ yield rate of ≈0.096 µg min^?1 at ?0.6 V versus RHE electrode in 0.25 m LiClO₄. During the electrochemical catalytic reaction, the crystal structure of FeS₂/CFP remains in the cubic pyrite phase, as analyzed by in situ X‐ray diffraction measurements. With near‐infrared laser irradiation (808 nm), the NH₃ yield rate of the FeS₂/CFP catalyst can be slightly improved to 0.1 µg min^?1 with high FE of 14.57%. Furthermore, density functional theory calculations demonstrate that the N₂ molecule has strong chemical adsorption energy on the iron atom of FeS₂. Overall, iron pyrite‐based materials have proven to be a potential electrocatalyst with photoactive behavior for ammonia production in practical applications.     

伪标签置信选择的半监督集成学习视频语义检测

在视频语义检测中，有标记样本不足会严重影响检测的性能，而且伪标签样本中的噪声也会导致集成学习基分类器性能提升不足。为此，提出一种伪标签置信选择的半监督集成学习算法。首先，在三个不同的特征空间上训练出三个基分类器，得到基分类器的标签矢量；然后，引入加权融合样本所属某个类别的最大概率与次大概率的误差和样本所属某个类别的最大概率与样本所属其他各类别的平均概率的误差，作为基分类器的标签置信度，并融合标签矢量和标签置信度得到样本的伪标签和集成置信度；接着，选择集成置信度高的样本加入到有标签的样本集，迭代训练基分类器；最后，采用训练好的基分类器集成协作检测视频语义概念。该算法在实验数据集UCF11上的平均准确率到达了83.48%，与Co-KNN-SVM算法相比，平均准确率提高了3.48个百分点。该算法选择的伪标签能体现样本所属类别与其他类别的总体差异性，又能体现所属类别的唯一性，可减少利用伪标签样本的风险，有效提高视频语义概念检测的准确率。     

土壤重金属光谱检测方法的应用研究

针对土壤重金属,在简述其危害的基础上,对其光谱检测方法具体应用进行深入分析,以此为实际的重金属检测工作提供理论参考,保证检测结果准确性与可靠性。