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Multi-heterointerfaces for selective and efficient urea production

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National science Review 2023年第2期10卷 212-223页

作者： Danyan Zhang Yurui Xue Xuchen Zheng Chao Zhang Yuliang Li Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of sciences Shandong Provincial Key Laboratory for science of material creation and energy conversion Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringShandong University

A major impediment to industrial urea synthesis is the lack of catalysts with high selectivity and activity,which inhibits the efficient industrial production of urea.Here,we report a new catalyst system suitable for the highly selective synthesis of industrial urea by in situ growth of graphdiyne on the surface of cobalt-nickel mixed oxides.Such a catalyst is a multi-heterojunction interfacial structure resulting in the obvious incomplete charge-transfer phenomenon between a graphdiyne and metal oxide interface and multiple intermolecular interactions.These intrinsic characteristics are the origin of the high performance of the catalyst.Studies on the me chanism reve al that the catalyst could effectively optimize the adsorption/desorption capacities of the intermediate and promote direct C-N coupling by significantly suppressing by-product reactions toward the formation of H2,CO,N2and NH3.The catalyst can selectively synthesize urea directly from nitrite and carbon dioxide in water at room temperature and pressure,and exhibits a record-high Faradaic efficiency of 64.3%,nitrogen selectivity(Nurea-selectivity) of86.0%,carbon selectivity(Curea-selectivity) of ～100%,as well as urea yield rates of 913.2 μg h-1mgcat-1and remarkable long-term stability.

关键词： porous materials carbon materials multi-heterointerfaces urea synthesis high-performance conversion

光响应有机模块自组装导致的氧自由基转化及其光催化应用

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science China materials 2024年第3期67卷 833-841页

作者：姚娴雅于胜胜张荣震王发栋刘辉牛凯凯邢令宝李培洲 School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 255000China School of Chemistry and Chemical Engineering Shandong Provincial Key Laboratory for Science of Material Creation and Energy ConversionScience Center for Material Creation and Energy ConversionInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100China

在光催化反应中实现对活性氧物种的单线态氧和超氧阴离子自由基的有效控制仍然是一个巨大挑战.本工作报道了一个从光敏模块构筑主客体超分子有机框架(SOF)策略,有效地实现了单线态氧到超氧阴离子自由基的转化.该TPA-BP-SOF结构中的光敏... 详细信息

在光催化反应中实现对活性氧物种的单线态氧和超氧阴离子自由基的有效控制仍然是一个巨大挑战.本工作报道了一个从光敏模块构筑主客体超分子有机框架(SOF)策略,有效地实现了单线态氧到超氧阴离子自由基的转化.该TPA-BP-SOF结构中的光敏模块由四个4,4′-联吡啶盐(BP)单元修饰的苯基桥接双(三苯胺)衍生物(TPA-BP)构成.来自于不同的TPA-BP中的两个BP单元通过与葫芦[8]脲(CB[8])发生首尾相连的强络合作用,形成了具有周期性孔结构和均匀溶解度的二维超分子有机框架纳米片结构.与单体TPA-BP中检测到的生成单线态氧的能量转移机制不同,通过主客体相互作用形成的TPA-BP-SOF能够有效促进电子转移高效产生超氧阴离子自由基.同时,该TPA-BP-SOF生成的超氧阴离子自由基能有效地用于水相芳基硼酸的氧化羟基化和N-苯基四氢异喹啉的氧化,收率分别高达88%和83%.本研究提出了一种利用SOF实现II型光敏剂向I型光敏剂有效转化的新方法,成功展示了其在光催化有机转化中的实际应用.

关键词： photocatalysis reactive oxygen species singlet oxygen supramolecular organic frameworks superoxide radical

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Recent Progress in Design of Organic Electro-optic materials with Ultrahigh Electro-optic Activities

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Chinese Journal of Chemistry 2022年第24期40卷 3001-3012页

作者： Huajun Xu Yanna Sun Yuanyuan Kan Ke Gao Science Center for Material Creation and Energy Conversion Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdaoShandong266237 China

Rationally designed organic electro-optic (OEO) materials demonstrate ultra-large electro-optic (EO) activities, affording inorganic-organic hybrid photonic devices with low drive voltage, large bandwidth, low energy consumption, and small footprint. OEO materials hold the potential to achieve EO coefficients (r_(33)) over 1000 pm/V. Over the past decade, however, the best performance of OEO materials is limited to 300—600 pm·V^(−1). This is partly because of the concern of increasing dipole moment and optical loss due to the redshifted absorbance of high hyperpolarizability chromophores. Recent advance of theory-guided design enables the OEO materials to achieve greatly enhanced hyperpolarizability and EO activity with dipole moment and propagation loss within acceptable constraints. Simultaneously, progress in hybrid device designs has greatly shortened the length of modulating waveguide, which resulted in significantly reduced sensitivity to propagation loss from redshifted absorption of OEO materials. Driven by theory-guided design method, several high-performance OEO materials have been presented with greatly enhanced EO coefficients beyond 1000 pm·V^(−1). This brief review summarizes the strategies to improve the EO activity including molecular engineering and hyperpolarizability, highlights the recent great progress in design of high-performance OEO materials, and discusses the problems needed to be solved in application for current OEO materials.

关键词： Nonlinear optics Chromophores Donor-acceptor systems Electro optic materials Electro-optic Modulator

Single-junction organic solar cell smashes performance record

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science China materials 2022年第9期65卷 2609-2610页

作者： Yanna Sun Huajun Xu Yuanyuan Kan Ke Gao Science Center for Material Creation and Energy Conversion Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237China

Organic solar cells(OSCs)have become a major focus in the field of the third-generation renewable energy thanks to their outstanding advantages of low cost,light weight and flexibility.In recent years,efforts dedicated to OSCs via material design,morphology optimization,and mechanism analysis have made remarkable progress,with power conversion efficiency(PCE)exceeding 19%.However,compared with inorganic solar cells(e.g.,Si or perovskite),the performance of OSCs remains limited by non-ideal exciton and charge transport.

关键词： exceeding performance record

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Ir0/graphdiyne atomic interface for selective epoxidation

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National science Review 2023年第8期10卷 173-179页

作者： Zhiqiang Zheng Lu Qi Yaqi Gao Xiaoyu Luan Yurui Xue Feng He Yuliang Li Shandong Provincial Key Laboratory for science of material creation and energy conversion Science Center for Material Creation and Energy Conversion School of Chemistry and Chemical EngineeringShandong University CAS Key Laboratory of Organic Solids Institute of ChemistryChinese Academy of Sciences School of Chemical sciences University of Chinese Academy of Sciences

The development of catalysts that can selectively and efficiently promote the alkene epoxidation at ambient temperatures and pressures is an important promising path to renewable synthesis of various chemical products. Here we report a new type of zerovalent atom catalysts comprised of zerovalent Ir atoms highly dispersed and anchored on graphdiyne(Ir0/GDY) wherein the Ir0is stabilized by the incomplete charge transfer effect and the confined effect of GDY natural cavity. The Ir0/GDY can selectively and efficiently produce styrene oxides(SO) by electro-oxidizing styrene(ST) in aqueous solutions at ambient temperatures and pressures with high conversion efficiency of ～100%, high SO selectivity of 85.5%, and high Faradaic efficiency(FE) of 55%. Experimental and density functional theory(DFT) calculation results show that the intrinsic activity and stability due to the incomplete charge transfer between Ir0and GDY effectively promoted the electron exchange between the catalyst and reactant molecule, and realized the selective epoxidation of ST to SO. Studies of the reaction mechanism demonstrate that Ir0/GDY proceeds a distinctive pathway for highly selective and active alkene-to-epoxide conversion from the traditional processes. This work presents a new example of constructing zerovalent metal atoms within the GDY matrix toward selective electrocatalytic epoxidation.

关键词： graphdiyne atom catalyst atomic interface selective epoxidation high-performance

Recent Progress in All-Solution-Processed Organic Solar Cells

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Chinese Journal of Chemistry 2024年第2期42卷 190-198页

作者： Yixuan Xu Qian Wang Wentao Zou Xu Zhang Yanna Sun Yuanyuan Kan Ping Cai Ke Gao School of materials science and Engineering&Guangxi Key Laboratory of Information materials Guilin University of Electronic TechnologyGuilinGuangxi 541004China Shandong Provincial Key Laboratory for science of material creation and energy conversion Science Center for Material Creation and Energy ConversionInstitute of Frontier and Interdisciplinary ScienceShandong UniversityQingdaoShandong 266237China

All-solution-processed organic solar cells(OSCs)(from the bottom electrode to the top electrode)are highly attractive thanks to their low cost,lightweight and high-throughput production.However,achieving highly efficient all-solution-processed OSCs remains a significant challenge.One of the key issues is the lack of high-quality solution-processed electrode systems that can replace indium tin oxide(ITO)and vacuum-deposited metal electrodes.In this paper,we comprehensively review recent advances in all-solution-processed osCs,and classified the devices as the top electrode materials,including silver nanowires(AgNWs),conducting polymers and composite conducting materials.The correlation between electrode materials,properties of electrodes,and device performance in all-solution-processed OSCs is elucidated.In addition,the critical roles of the active layer and interface layer are also discussed.Finally,the prospects and challenges of all-solution-processed OSCs are presented.

关键词： Organic solar cells All-solution-processed organic solar cells Solution-processed electrodes High performance Silver nanowires Conductive polymers Composite conducting materials

Multifunctional Spacer Cations for In-situ Formation of Two-dimensional Passivation Layer in Efficient Perovskite Solar Cells

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Multifunctional Spacer Cations for In-situ Formation of Two-...

Enhanced Performance via π-Bridge Alteration of Porphyrin-Based Donors for All-Small-Molecule Organic Solar Cells

第十届新型太阳能材料科学与技术学术研讨会

作者： Le Liu Tonggang Jiu Shandong Provincial Key Laboratory for science of material creation and energy conversion Science Center for Material Creation and Energy ConversionInstitute of Frontier and Interdisciplinary ScienceShandong University

Surface passivation via two-dimensional(2D) perovskite is critical for perovskite solar cells to achieve remarkable performances,in which the applied spacer cations of 2D perovskite play an important role on structural templating.In our works,firstly,we demonstrate cyclopropylcarbamidine hydrochloride(CPAH) as a novel organic halide salt to construct 2D layer for surface passivation of phase-pure FAPbI film.The results verify that the introduction of 2D passivation layer is beneficial to the suppression of charge recombination and the promotion of charge transfer,which contributes an optimal voltage loss of 0.34 eV.Meanwhile,4-chlorobenzamidine hydrochloride(CBAH) is developed as a spacer to form orientationally crystallized nanorod-like 1D perovskite on the top surface of 3D perovskite for surface passivation of FAPbI perovskite.Moreover,a multiple nitrogen sites contained organic spacer molecule(1H-Pyrazole-1-carboxamidine hydrochloride,PAH) is introduced to form 2D passivation layer on the surface of FAPbI based perovskite.Interestingly,the 2D perovskite nanosheets are found to grow with a direction perpendicular to the substrate due to the multiple-site intermolecular interactions,which promotes charge transfer and decreases energy loss.Therefore,an impressive power conversion efficiency of 24.6% and outstanding long-term stability is achieved for the as-prepared 2D/3D perovskite devices.

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Chinese Journal of Chemistry 2023年第6期41卷 644-650页

作者： Haojiang Shen Yi Ren Jianfeng Li Yixuan Xu Chenyang Han Wentao Zou Huajun Xu Yanna Sun Yuanyuan Kan Ke Gao School of materials science and Engineering Lanzhou Jiaotong UniversityLanzhouGansu 730070China Science Center for Material Creation and Energy Conversion Institute of Frontier and Interdisciplinary ScienceShandong University QingdaoShandong266237China

All-small-molecule organic solar cells (ASM OSCs) are promising for commercial application due to the well-defined chemical structures, convenient purifying process and low batch-to-batch variation. However, the similarity of molecule structures between small molecule donors and acceptors makes a hard regulation of their blend morphology, which will limit the efficiency.

关键词： All-small-molecule organic solar cells Porphyrin-based small molecule donor Binary device π-bridge engineering Morphology tuning

吡嗪基共价有机框架的内表面磺化作用显著增强质子传导性

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science China materials 2024年第1期67卷 125-133页

作者：栾天翔王秋荣张鹏图李万超孔硕冯祎静苑世领李培洲 School of Chemistry and Chemical Engineering Shandong Provincial Key Laboratory for Science of Material Creation and Energy ConversionScience Centre for Material Creation and Energy ConversionInstitute of Frontier and Interdisciplinary ScienceShandong UniversityJinan 250100China School of Chemical Engineering Shandong Institute of Pertroleum and Chemical TechnologyDongying 257061China No.1 Institute of Geology and Mineral Resources of Shandong Province Jinan 250100China

通过表面改性方法以提高电解质的质子传导性和长寿命使用性是制造高效质子传导电解质的可行方法.本文以吡嗪基共价有机框架(CS-COF)作为模板,构建了其叔丁基缺失的COF结构,命名为PyHATP-1.研究发现,在353 K和98%相对湿度条件下,磺化样品... 详细信息

通过表面改性方法以提高电解质的质子传导性和长寿命使用性是制造高效质子传导电解质的可行方法.本文以吡嗪基共价有机框架(CS-COF)作为模板,构建了其叔丁基缺失的COF结构,命名为PyHATP-1.研究发现,在353 K和98%相对湿度条件下,磺化样品PyHATP-1-SO_(3)H的质子电导率从PyHATP-1的7.2×10^(-6)S cm^(-1)指数级提高到了1.3×10^(-3)S cm^(-1).此外,在骨架中加入磷酸分子后,磺化的H_(3)PO_(4)@PyHATP-1-SO_(3)H不仅比未磺化的H_(3)PO_(4)@PyHATP-1(2.0×10^(-3)S cm^(-1))具有显著提高的质子传导性(0.88×10^(-1)S cm^(-1)),而且表现出更佳的重复使用性.接触角测试和密度泛函理论计算表明,其质子传导性的显著增强和长寿命重复使用性应归功于孔隙表面的后磺化修饰,这大大提高了对质子载体(水和磷酸分子)的亲和力.这项研究表明,通过改变多孔材料的固有表面性质,可以获得具有高质子电导率和长寿命重复使用性的质子传导电解质.

关键词：密度泛函理论计算可行方法质子电导率重复使用性质子传导表面性质共价有机框架多孔材料

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