摘要：人工光合成通过模拟自然界的光合作用合成人类必须的化学品,并在光解水制氢、水和氧气反应制备双氧水等领域得到了广泛的关注.然而,双氧水不稳定导致产物的分离和提纯成本高,阻碍了其进一步发展.为解决上述问题,最近,南京理工大学张侃教授团队联合韩国延世大学Jong Hyeok Park教授,河海大学敖燕辉教授开发出了基于人工树叶的自循环光芬顿系统,在碳酸氢盐溶液和微量Mn^(2+)/Mn^(4+)的协同作用下,成功地将原位生产的双氧水进一步生成活性含氧物种(ROSs)并用于污水处理,实现了高效太阳能驱动H_(2)O_(2)的原位生产与利用(见***.,2022,13,4982).该工作首先利用人工树叶阴极部分对Mn^(4+)离子还原,实现了Mn^(2+)/Mn^(4+)氧化还原物种在催化体系中的循环使用,确保了芬顿体系的可持续性.其次,通过对耦合的光阳极以及阴极的表面动力学过程进行优化,构建了太阳能到双氧水转换效率超过1.46%的人工树叶.实验发现,70 cm^(2)的大面积器件可在70 min内矿化含有5 ppm罗丹明B,5 ppm亚甲基蓝和5 ppm对硝基苯酚的混合污水,并表现出超过一个月的稳定性.综上,本文可为发展新的太阳能驱动环境处理模式提供借鉴.

摘要：工业化无疑促进了经济的发展,提高了生活水平,但也导致了一些问题,包括能源危机、环境污染、全球变暖等,其中这些所产生问题主要是由燃烧煤炭、石油和天然气等化石燃料引起的。光催化技术具有利用太阳能将二氧化碳转化为碳氢化合物燃料、从水中制氢、降解污染物等优点,从而在解决能源危机的同时避免环境污染,因此被认为是解决这些问题的最有潜力的技术之一。在各种光催化剂中,碳化硅(SiC)由于其优良的电学性能和光电化学性质,在光催化、光电催化、电催化等领域具有广阔的应用前景。本文首先系统地阐述了各种SiC的合成方法,具体包括模板生长法、溶胶凝胶法、有机前驱物热解法、溶剂热合成法、电弧放电法,碳热还原法和静电纺丝等方法。然后详细地总结了提升SiC光催化活性的各种改性策略,如元素掺杂、构建Z型(S型)体系、负载助催化剂、可见光敏化、构建半导体异质结、负载炭材料、构建纳米结构等。最后重点论述了半导体的光催化机理以及SiC复合物在光催化产氢、污染物降解和CO_(2)还原等领域的应用研究进展,并提出了前景展望。

摘要：Conjugated covalent organic frameworks(COFs)hold great promise in photocatalytic hydrogen evolution owing to their high crystallinity,large surface area,and distinct ***,COFs exhibit poor charge ***,investigating highly effective COF-based photocatalysts is *** the first time,conjugated COF/perylene diimide urea polymer(PUP)all-organic heterostructure with S-scheme interfacial charge-transfer channels was successfully developed and manufactured via in situ coupling of the two-dimensional triazine-based imine-linked COF(denoted as TATF-COF)with *** optimal photocatalytic hydrogen-evolution rate of 94.5 mmol h^(-1) g^(-1) for TATF-COF/PUP is 3.5 times that of pure TATF-COF and is comparable to or even higher than that of the previously reported COF-based photocatalysts,resulting in an apparent quantum efficiency of up to 19.7%at 420 *** improved directional S-scheme charge transfer driven by the tuned built-in electric field and enhanced oxidation and reduction reaction rates of the photogenerated carriers contribute synergistically to the boosted photocatalytic H_(2) *** and theoretical studies reveal plausible H_(2) evolution and spatial S-scheme charge-separation mechanisms under visible-light *** study provides advanced methods for constructing all-organic S-scheme high-efficiency photocatalysts by the modulation of band structures.

摘要：Single-atom catalysts(SACs)have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined *** tailored coordination with nitrogen atom,the metal-nitrogen(M-N)-based SACs have demonstrated interesting physical,optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past *** substantial efforts in constructing various M–N-based SACs,the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently ***,the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure,catalytic mechanism,single-metal atom(SMA)confinement and their photocatalytic and electrocatalytic activities(conversion,selectivity,stability and etc).Based on the analysis of fundamentals of M–N-based SACs,theoretical calculations and experimental investigations,including synthetic methods and characterization techniques,are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed ***,the challenges and perspectives for constructing highly active M–N based photocatalysis and electrocatalysis SACs are *** particular,extensive technical and mechanism aspects are thoroughly discussed,summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.

摘要：The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic ***,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling *** using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic ***,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) *** addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution *** showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS ***,the apparent quantum efficiency reached 12.0% at 450 *** is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.

摘要：课程思政是德育教育,是将思想政治教育在悄无声息中有机地融入教学的过程中,是教书育人的过程体现。课程思政是课程加思政,所以实施必然是以课程的基础理论知识为主轴,融入社会主义核心价值观的教育元素,构建配位化学课程思政教学体系。本文以配位化学第一章的教学设计为例,对思政案例进行初步的探讨。

摘要：宏观动力学研究和化工设计都是从反应速率方程开始,确定速率方程的首要任务是测定反应级数。以生活和科研中实际问题的解决为驱动,以小组为单位,结合探究性实验“电导率法测定乙酸乙酯皂化反应的反应级数”的PBL教学设计和实施,激发和引导学生通过自主学习、自主探究、合作学习的方式共同解决问题,掌握了积分法,提高了学生宏观动力学实验设计能力和理论联系实际能力,培养了学生勇于创新、善于合作的科研精神。

摘要：Noble metal cocatalysts have shown great potential in boosting the performance of CdS in photocatalytic water ***,the mechanism and kinetics of electron transfer in noble-metal-decorated CdS during practical hydrogen evolution is not clearly ***,Pt-nanoparticle-decorated CdS nanorods(CdS/Pt)are utilized as the model system to analyze the electron transfer kinetics in CdS/Pt *** femtosecond transient absorption spectroscopy,three dominating exciton quenching pathways are observed and assigned to the trapping of photogenerated electrons at shallow states,recombination of free electrons and trapped holes,and radiative recombination of locally photogenerated electron-hole *** introduction of Pt cocatalyst can release the electrons trapped at the shallow states and construct an ultrafast electron transfer tunnel at the CdS/Pt *** CdS/Pt is dispersed in acetonitrile,the lifetime and rate for interfacial electron transfer are respectively calculated to be~5.5 ps and~3.5×10^(10) s^(−1).The CdS/Pt is again dispersed in water to simulate photocatalytic water *** lifetime of the interfacial electron transfer decreases to~5.1 ps and the electron transfer rate increases to~4.9×10^(10) s^(−1),confirming that Pt nanoparticles serve as the main active sites of hydrogen *** work reveals the role of Pt cocatalysts in enhancing the photocatalytic performance of CdS from the perspective of electron transfer kinetics.

摘要：Reducing CO_(2) to hydrocarbon fuels by solar irradiation provides a feasible channel for mitigating excessive CO_(2) emissions and addressing resource ***,severe charge recombi‐nation and the high energy barrier for CO_(2) photoreduction on the surface of photocatalysts com‐promise the catalytic ***,a 2D/2D Bi_(2)MoO_(6)/BiOI composite was fabricated to achieve improved CO_(2) photoreduction *** transfer in the composite was facilitated by the van der Waals heterojunction with a large‐area *** function calculation demon‐strated that S‐scheme charge transfer is operative in the composite,and effective charge separation and strong redox capability were revealed by time‐resolved photoluminescence and electron para‐magnetic resonance ***,the intermediates of CO_(2) photoreduction were identi‐fied based on the in situ diffuse reflectance infrared Fourier‐transform *** functional theory calculations showed that CO_(2) hydrogenation is the rate‐determining step for yielding CH_(4) and *** Bi_(2)MoO_(6) into the composite further decreased the energy barrier for CO_(2) photoreduction on BiOI by 0.35 *** study verifies the synergistic effect of the S‐scheme heterojunction and van der Waals heterojunction in the 2D/2D composite.

摘要：以葛根为原料，用CO2超临界提取法提取葛根中的葛根素，考查了提取温度、提取时间、料液比和萃取压力对葛根素提取率的影响。实验结果表明：在提取温度为50℃，料液比为300：350（g／mL），萃取压力为35MPa条件下萃取2h，葛根素的提取率为0．1183％。