摘要：The energy crisis and global warming become severe issues. Solar-driven CO2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical（PEC） process,which can integrate the merits of both photocatalysis and electrocatalysis, boosts splendid talent for CO2 reduction with high efficiency and excellent selectivity. Recent several decades have witnessed the overwhelming development of PEC CO2 reduction. In this review, we attempt to systematically summarize the recent advanced design for PEC CO2 reduction. On account of basic principles and evaluation parameters, we firstly highlight the subtle construction for photocathodes to enhance the efficiency and selectivity of CO2 reduction, which includes the strategies for improving light utilization, supplying catalytic active sites and steering reaction ***, diversiform novel PEC setups are also *** exploited setups endow a bright window to surmount the intrinsic disadvantages of photocathode, showing promising potentials for future applications. Finally, we underline the challenges and key factors for the further development of PEC CO2 reduction that would enable more efficient designs for setups and deepen systematic understanding for mechanisms.

摘要：金属纳米晶体具有独特的表面等离激元特性,为太阳能转换成化学能提供了新的机遇。本文以课题组近期的研究工作为例,阐述在催化有机加氢反应中表面等离激元效应所产生的多种物理过程的作用机制。该系列工作实现了太阳能向化学能的有效转换,为太阳能替代传统有机化工中的热催化提供了可能性,对等离激元催化材料的设计具有一定的指导意义。

摘要：21世纪以来,能源短缺和环境污染一直是人类面临的重大挑战。光催化二氧化碳(CO_(2))还原,通过半导体捕获光能,获得碳氢化合物太阳能燃料是解决能源危机并推动碳循环的有前景的策略之一。然而,活性低、产物选择性差又极大地限制了这一技术的实际应用。因此,调控产物选择性并提高光催化效率、加深对CO_(2)还原反应机理的理解具有重要意义。近年来,超薄材料以其较高的比表面积,丰富的不饱和配位的表面原子,较短的电荷从内部到表面的迁移路径,以及可裁剪的能带结构受到了广泛关注,并在光催化CO_(2)还原领域取得了可喜的成果。本文在总结光催化CO_(2)还原反应机理的基础上,介绍了通过构建异质结构、设计Z型系统、引入助催化剂以及缺陷工程等策略促进超薄纳米结构电子空穴分离和调控其电荷迁移路径的研究成果,并指出了提高光催化CO_(2)还原效率和优化产物选择性的发展前景与挑战。

摘要：Efficient tandem reactions on a single catalytic nanostructure would be beneficial to improving chemical transformation efficiency and reducing safety implications. It is imperative to identify the active sites for each single step reaction so that the entire reaction process can be optimized by designing and integrating the sites. Herein, hydrogen transfer reaction is taken as a proof-of-concept demonstration to show that the spatial integration of active sites is important to the catalytic efficiency of the entire process in tandem reactions. We identified specific active sites (i.e., various sites at faces versus corners and edges) for formic acid decomposition and alkene/nitrobenzene hydrogenation-the two steps in hydrogen transfer reactions, by employing three different shapes of Pd nanocrystals in tunable sizes. The investigation reveals that the decomposition of formic acid occurs preferentially at the edge sites of cubic nanocrystal and the plane sites of octahedral/ tetrahedral nanocrystals, while the hydrogenation takes place mainly at the edge sites of both cubic and octahedral/ tetrahedral nanocrystals. The consistency of active edge sites during different step reactions enables cubic nanocrystals to exhibit a higher activity than octahedral nanocrystals in hydrogen transfer reactions, although octahedrons offer comparable activities to cubes in formic acid decomposition and hydrogenation reactions. Guided by these findings, we further improved the overall performance of tandem catalysis by specifically promoting the limiting step through nanocatalyst design. This work provides insights into the rational design of heterogeneous nanocatalysts in tandem reactions.

摘要：Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high ***,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this *** electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m ***,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish *** splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and *** selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent *** work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.

摘要：新型磁性荧光材料的开发对鉴定和刑事侦查具有重要意义。由于传统相机中使用的光敏元件在500~700nm范围内表现出最高的量子效率,因此以507~533 nm、533~568 nm和637~683 nm为主发射峰的镧系上转换纳米粒子(UCNPs)适合用于构建磁性荧光材料。本文通过配体连接的方法证实了一种磁性上转换纳米颗粒—NaGdF_(4):Yb,Er-Fe_(3)O_(4)。在优化反应参数后,复合颗粒获得了优异的磁性能和上转换荧光强度,并且可在各种基底上实现高对比度的潜在指纹识别。得益于上转换发光与磁性的结合,指纹识别具有了高灵敏度与通用性。

摘要：Amidst the development of photoelectrochemical(PEC)CO_(2) conversion toward practical application,the production of high-value chemicals beyond C1 compounds under mild conditions is greatly desired yet ***,through rational PEC device design by combining Au-loaded and N-doped TiO_(2) plate nanoarray photoanode with Zn-doped Cu_(2)O dark cathode,efficient conversion of CO_(2) to CH3COOH has been achieved with an outstanding Faradaic efficiency up to 58.1%(91.5%carbon selectivity)at 0.5 V ***/*** programmed desorption and in situ Raman spectra reveal that the Zn-dopant in Cu_(2)O plays multiple roles in selective catalytic CO_(2) conversion,including local electronic structure manipulation and active site modification,which together promote the formation of intermediate*CH2/*CH3 for C-C *** from that,it is also unveiled that the sufficient electron density provided by the Au-loaded and N-doped TiO_(2) plate nanoarray photoanode plays an equally important role by initiating multi-electron CO_(2) *** work provides fresh insights into the PEC system design to reach the multi-electron reduction reaction and facilitate the C-C coupling reaction toward high-value multicarbon(C2+)chemical production via CO_(2) conversion.