摘要：Rationally manipulating the in‐situ formed catalytically active surface of catalysts remains a great challenge for a highly efficient water ***,we report a cationic oxidation method which can adjust the leaching of the in‐situ catalyst and promote the reconstruction of dynamic surface for the oxygen evolution reaction(OER).The chlorine doping can reduce the possibility of triggering in‐situ cobalt oxidation and chlorine leaching,leading to a transformation of the surface chlorine doped LaCoO_(3)(Cl‐LaCoO_(3))into an intricate amorphous(oxygen)hydroxide *** thus,Cl‐LaCoO_(3)nanocrystals shows an ultralow overpotential of 342 mV at the current density of 10 mA cm^(–2)and Tafel slope of 76.2 mV dec–*** reconstructed Cl‐LaCoO_(3)is better than many of the most advanced OER catalysts and has proven significant *** work provides a new prospect for designing a high‐efficiency electrocatalyst with optimized perovskite‐structure in renewable energy system.

摘要：Constructing a suitable heterojunction photocatalytic system from two photocatalytic materials is an efficient approach for designing extremely efficient photocatalysts for a broader range of environmental,medical,and energy ***,the construction of a step-scheme heterostructure system(hereafter called the S-scheme)has received widespread attention in the photocatalytic field due to its ability to achieve efficient photogenerated carrier separation and obtain strong photo-redox ***,a novel S-scheme heterojunction system consisting of 2D O-doped g-C_(3)N_(4)(OCN)nanosheets and 3D N-doped Nb_(2)O_(5)/C(N-NBO/C)nanoflowers is constructed via ultrasonication and vigorous agitation technique followed by heat treatment for the photocatalytic degradation of Rhodamine B(RhB).Detailed characterization and decomposition behaviour of RhB showed that the fabricated material shows excellent photocatalytic efficiency and stability towards RhB photodegradation under visible-light *** enhanced performance could be attributed to the following factors:fast charge transfer,highly-efficient charge separation,extended lifetime of photoinduced charge carriers,and the high redox capability of the photoinduced charges in the S-scheme *** trapping experiment conditions and electron paramagnetic resonance provide clear evidence of the S-scheme photogenerated charge transfer path,meanwhile,the RhB mineralization degradation pathway was also investigated using *** study presents an approach to constructing Nb_(2)O_(5)-based S-scheme heterojunctions for photocatalytic applications.

摘要：太阳能蒸发是一种可持续的高盐废水处理技术,然而运行中蒸发器表面的盐积累会严重缩短蒸发器的寿命.如何使蒸发器兼具高蒸发效率和良好拒盐性是目前面临的挑战.本研究设计了一种三维碳纳米纤维/氧化石墨烯复合气凝胶(CNF/GOA).氧化石墨烯的引入不仅增强了CNF/GOA的力学性能,同时构建了丰富的分级互连孔道结构,加快了水的传输和盐的扩散,实现了高蒸发速率和良好的拒盐性.此外,通过调控CNF/GOA的浸没深度和孔道结构,抑制了水的热传导损失,降低了水的蒸发焓,在一个太阳照射下实现了3.47 kg m^(-2)h^(−1)的蒸发速率.更重要的是,即使处理高盐水,蒸发器表面也没有产生任何盐结晶.长期实验和户外脱硫废水蒸发实验表明,CNF/GOA具有良好的实际应用前景.

摘要：局部电荷的强离域和强偶极矩是影响共价有机框架(COFs)基光催化剂催化析氢性能的两个关键因素.然而,基于精确的调控结构模型来系统研究这种构效关系的报告相对较少.本研究提出了一种新的策略,通过合理的设计,制备了三种三芴酮基COFs,通过在分子水平上调控单体的结构和偶极来提高局部电荷离域指数.我们重点研究这三种三芴酮基COF的局部电荷离域与光催化性能之间的构效关系.在不同三芴酮基COF中,1,3,5-三(对甲酰基苯基)苯基COF(TeTpb-COF)展现出21.6 mmol g^(-1)h^(-1)的最高析氢速率,与2,4,6-三(4-醛基苯基)-1,3,5-三嗪基COF(TeTt-COF,0.2mmol g^(-1)h^(-1))相比,光催化析氢性能提高了108倍.这种性能的增强可归因于其强大的分子内置电场提高了供体-受体嵌段单元中光生电荷的有效分离效率.这项工作证实了调整构建块可以极大增强三芴酮基COFs中的局部偶极矩,从而显著改善光催化析氢性能.构建模块的调控策略为创建高效的新型COF基光催化析氢平台提供了新机会.

摘要：当前,高渗透性反渗透膜材料的研究引起了广泛的关注,然而高渗透导致的浓差极化与膜污染加剧等瓶颈问题限制了高性能膜材料的应用发展.本工作采用机器学习结合超级计算提出了针对先进反渗透膜材料的组件进水隔网(亚毫米级)与系统(米级)的多尺度优化设计新方法.在进料含盐度35,000 ppm,回收率50%典型工况下,对标目前国际先进海水反渗透淡化工艺,本文提出的优化方案能使淡水制备比能耗(1.66 k Wh/m^(3))降低27.5%,所需膜面积减少约37.2%,系统最大浓差极化因子控制在工程允许范围以内(<1.20),可有效缓解高渗透膜系统中膜污染问题,为高性能膜材料精准设计提供理论依据、计算工具和大数据支撑,有重要的应用潜力.本文提出的机器学习结合超算的多尺度设计新研究范式,突破了基于“试错法”的传统单一尺度组件设计限制,高通量并行计算规模可扩展至93,120核以上,较串行算法计算效率提升3000倍以上,可大幅度缩短高性能膜组件的设计周期.

摘要：The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption *** triazine frameworks(CTFs),emerged as a class of crystalline covalent organic frameworks(COFs),have been widely examined for various separation applications,owing to their large porosity,high stability,and rich nitrogen(N)*** development of CTFs for efficient adsorption of mercury(Ⅱ)(Hg^(2+))is of great importance for the field,whereas it is rarely attempted,on account of limited synthetic strategies and unknown structural-property relations of conventional CTFs derived from ionothermal ***,we report rational synthesis of a crystalline CTF with methylthio pendant arms for efficient removal of Hg^(2+)with an exceptional capacity of 751 mg·g^(-1),ranking at the top among previously-reported *** work may open up new possibility in the synthesis of COFs for various separations.