摘要：Aqueous zinc ion hybrid capacitors(ZIHCs)are considered one of the most promising electrochemical energy storage systems due to their high safety,environmental friendliness,low cost,and high power ***,the low energy density and the lack of sustainable design strategies for the cathodes hinder the practical application of ***,we design the N and O co-doped porous carbon cathode by annealing metal-organic framework(ZIF-8).ZIF-8 retains the original dodecahedral structure with a high specific surface(2814.67 m^(2)/g)and I_(G)/I_(D) ratio of 1.0 during carbonization and achieves self-doping of N and O *** defect sites are introduced into the porous carbon to provide additional active sites for ion adsorption after the activation of carbonized ZIF-8 by KOH *** ZIHCs assembled with modified ZIF-8 as the cathode and commercial zinc foil as the anode show an energy density of 125 W∙h/kg and a power density of 79 W/*** addition,this ZIHCs device achieves capacity retention of 77.8%after 9000 electrochemical cycles,which is attributed to the diverse pore structure and plentiful defect sites of ZIF-8-800(KOH).The proposed strategy may be useful in developing high-performance metal-ion hybrid capacitors for large-scale energy storage.

摘要：With the strict control of sulfur content in fuels,oxidative desulfurization(ODS),a promising desulphurization technology,needs to be continuously *** this study,we integrated multiple approaches(fabricating a porous structure,increasing phosphomolybdic acid(PMo)loading,improving amphiphilicity,and enhancing the intrinsic activity of PMo using a reductive framework)into PAF-54 carriers to improve ODS catalytic *** catalytic performance suggested that PAF-54 was not simply used as a carrier for PMo by physical *** the binding process,electron transfer between PAF-54 and PMo formed Mo^(5+)with superior catalytic *** to the presence of PAF-54,the catalytic activity of PMo as the active component qualitatively improved to achieve rapid and efficient *** importantly,we found that other nitrogen-rich porous organic polymers can also reduce some of Mo^(6+)in PMo during loading,and its formation mechanism was *** work provides a feasible strategy for designing highly efficient DOS catalysts.

摘要：Efficient multi-resonance thermally activated delayed fluorescence(MR-TADF)materials hold significant potential for applications in organic light-emitting diodes(OLEDs)and ultra-high-definition ***,the stringent synthesis conditions and low yields typically associated with these materials pose substantial challenges for their practical *** this study,we introduce an innovative strategy that involves peripheral modification with sulfur and selenium atoms for two materials,CFDBNS and *** approach enables a directed one-shot borylation process,achieving synthesis yields of 66%and 25%,respectively,while also enhancing reverse intersystem crossing *** emitters exhibit ultra-narrowband sky-blue emissions centered around 474 nm,with full width at half maximum(FWHM)values as narrow as 19 nm in dilute toluene solutions,along with high photoluminescence quantum yields of 98%and 99%in doped films,*** OLEDs based on CFDBNS and CFDBNSe display sky-blue emissions with peaks at 476 and 477 nm and exceptionally slender FWHM values of 23 ***,the devices demonstrate remarkable performances,achieving maximum external quantum efficiencies of 24.1%and 27.2%.This work presents a novel and straightforward approach for the incorporation of heavy atoms,facilitating the rapid construction of efficient MR-TADF materials for OLEDs.

摘要：J-aggregates of cyanine have shown great merits in tumor photothermal therapy(PTT)due to their distinct redshift absorption as well as superior photothermal conversion efficiency(PCE).However,due to the complexity of intermolecular interactions,especially the impact of steric hindrance on aggregation,exploring effective strategies to regulate the aggregation modes of organic materials remains ***,steric hindrance-regulated J-aggregation of near-infrared(NIR)cyanine was reported based on Pt-coordinated cyanine self-assembly with unexpected“butterfly effect”.Two Pt-coordinated cyanine dimers CyR-Pt(R=Me and Et)were synthesized and spontaneously self-assembled into aggregates in aqueous ***-Pt aggregates were loose and amorphous *** replacing ethyl with methyl to reduce steric hindrance,a tiny change resulted in the generation of tightly stacked cyanine J-aggregates(thickness less than 3 nm)observed in CyMe-Pt ***,this unexpected“butterfly effect”enabled CyMe-Pt J-aggregates to effectively inhibit reactive oxygen species and greatly improve its ***,CyMe-Pt J-aggregates with NIR-II absorption exhibited outstanding photothermal stability and higher PCE(η=37%)than CyEt-Pt disordered aggregates(η=20%).Evident tumor suppression performance of CyMe-Pt J-aggregates was validated under 980 nm laser irradiation,demonstrating its great potential in tumor PTT.

摘要：光催化CO_(2)还原合成太阳能燃料对缓解CO_(2)排放引起的全球变暖和降低化石燃料消耗具有重要意义.然而,目前的光催化剂仍然存在反应动力学缓慢和选择性不理想的问题,特别是对于C_(2+)产物的生成,极大地限制了光催化的工业化进程.过去几十年中,关于太阳能驱动的CO_(2)还原的研究展示出鼓舞人心的结果,包括活性位点的构建.本综述重点介绍了通过构建活性位点制备原子级分散催化剂在光催化CO_(2)还原中的最新进展,包括两个独立的活性位点、成对双活性位点和基于活性位点构型的纳米团簇.此外,详细讨论了CO_(2)在活性位点上的活化机制和表征方法.特别是考虑到实验研究与实际应用之间的差距,整合实验和理论的结果,以实现潜在的结构-活性关系和高目标产物选择性发展.最后,概述了该领域存在的挑战,并展望了活性位点的合理设计和机理研究.

摘要：调控铂(Pt)电子结构是增强Pt基电催化剂活性和耐久性的关键策略.本研究开发了CeO_(2)/PtBi金属间纳米板(NPs),这种结构通过Pt和Bi之间的强p-d轨道杂化,显著提高了催化剂在甲醇电氧化反应(MOR)中的活性和稳定性.CeO_(2)的表面沉积不仅进一步优化了Pt的电子结构,还提供了额外的羟基吸附位点.特别是,在酸性和碱性环境下,CeO_(2)/PtBi NPs展现出超越商业Pt/C的甲醇电氧化质量活性,分别提高了1.62和7.65倍.在经历了1000次耐久性测试后,CeO_(2)/PtBi NPs在酸碱环境下的活性仅分别下降了20.1%和39.8%,相比之下,商业Pt/C的活性在相同条件下分别下降了55.4%和78.5%.CeO_(2)/PtBi NPs的这一卓越性能得益于Pt与Bi之间的p-d轨道杂化以及CeO_(2)表面工程对催化剂电子结构的有效调节.本研究为Pt基电催化剂设计提供了新的电子结构调控策略和深入见解.

摘要：Herein,two asymmetric hexacyclic fused small molecule acceptors(SMAs),namely BP4F-HU and BP4F-UU,were *** elongated outside chains in the BP4F-UU molecule played a crucial role in optimizing the morphology of blend film,thereby improving charge mobility and reducing energy loss within the corresponding ***,the PM6:BP4F-UU device exhibited a higher open-circuit voltage(V_(oc))of 0.878 V compared to the PM6:BP4F-HU device with a V_(oc)of 0.863 ***,a new wide bandgap SMA named BTP-TA was designed and synthesized as the third component to the PM6:BP4F-UU host binary devices,which showed an ideal complementary absorption spectrum in PM6:BP4F-UU *** addition,BTP-TA can achieve efficient intermolecular energy transfer to BP4F-UU by fluorescence resonance energy transfer(FRET)pathway,due to the good overlap between the photoluminescence(PL)spectrum of BTP-TA and the absorption region of ***,ternary devices with 15wt%BTP-TA exhibits broader photon utilization,optimal blend morphology,and reduced charge recombination compared to the corresponding binary ***,PM6:BP4F-UU:BTP-TA ternary device achieved an optimal power conversion efficiency(PCE)of 17.83%with simultaneously increased V_(oc)of 0.905 V,short-circuit current density(J_(sc))of 26.14 mA/cm^(2),and fill factor(FF)of 75.38%.

摘要：近红外(NIR)光驱动水分解产生氢气(H_(2))一直以来都是光催化领域备受关注的问题,但由于其动力学和热力学方面的缺陷,迄今为止仍是一项艰巨的挑战.为了突破这一限制,我们通过简便的水热法设计出了富含硫空位的无贵金属二维(2D)ZnIn_(2)S_(4)-基光催化剂,并首次使用单组分ZnIn_(2)S_(4)-基材料实现了波长大于800 nm的近红外驱动制氢性能.根据价带光谱、紫外-可见-近红外DRS光谱、稳态PL光谱、瞬态光电流响应和EPR表征,我们揭示了存在一个高效的Urbach带尾吸收用于捕获近红外光.硫空位在ZnIn_(2)S_(4)纳米片中的成功构建不仅扩展了光谱吸收范围,而且具有出色的载流子扩散特性和丰富的活性位点.因此,我们的研究结果可能会为未来开发近红外响应的ZnIn_(2)S_(4)-基光催化剂用于实现高效近红外驱动制氢提供一定的指导.

摘要：石墨炔由于其高载流子迁移率和有序的孔隙结构被认为是一种很有应用前景的光催化材料.本研究通过交叉偶联合成了一种新型球状石墨炔,并与棒状Mn_(0.2)Cd_(0.8)S耦合构建了S型异质结用于光催化析氢.结果表明,Mn_(0.2)Cd_(0.8)S/石墨炔异质结光催化剂表现出优异的光催化活性,产氢性能分别较Mn_(0.2)Cd_(0.8)S和球形石墨炔单体催化剂提升了16.78和613.2倍.同时,该催化剂应用于平米级规模产氢取得较好效果.其优异的光催化活性可归因于石墨炔的独特性能及S-scheme异质结的有效构建.通过紫外光电子能谱、原位辐射X射线光电子能谱、电子顺磁共振能谱、密度泛函理论计算和其他表征技术探究了S-scheme异质结的形成和光催化活性的增强.该工作可为石墨炔的形貌可调性制备以及高效异质结光催化剂的设计和合成提供新参考.

摘要：由于析氧反应的内在动力学缓慢,开发高效的光催化析氧反应催化剂,以利用太阳能进行光催化分解水产氧,面临着巨大的挑战.本研究设计了一种新型的“主-客体”光催化系统,通过简单的预负载将单位点钌(Ru)分子催化剂引入共价三嗪框架(CTFs)的孔道内.其中,CTFs作为光敏剂和光催化载体,单核钌配合物Ru-bda-Isoq作为分子水氧化催化剂.在可见光照射下,Ru-bda-Isoq@CTF-Bph在5h内平均析氧速率达到2308μmol g^(-1)h^(-1),其性能超过了大多数有机光催化剂.同时,研究还发现多孔光敏剂与分子催化剂之间的结构匹配起着非常关键的作用.该体系具有广泛的适用性,这一策略有助于高效水氧化光催化系统的设计.