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Unraveling post-growth mechanisms of monolayer CsPbBr3 nanocubes:Laser-enhanced transformations and cathodoluminescence-electron microscopy correlations

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Journal of Energy Chemistry 2025年第1期100卷 146-156页

作者： Mingxing Li Xiaoge Wang Xiaofan Cao Zhiqun He Chunjun Liang Mingxing Chen Jing Ju Fangtian You Key Laboratory of Luminescence and Optical Information Ministry of Education Institute of Optoelectronic Technology Beijing Jiaotong University Beijing National Laboratory for Molecular Sciences (bnlms) College of Chemistry and Molecular Engineering Peking University

Lead-halide perovskite nanoparticles（LHP NPs） are highly promising materials for next-generation displays and solid-state lighting due to their exceptional optical properties. However, their inherent instability presents a significant challenge. Recent advances have demonstrated that optoelectronic devices based on monolayer nanoparticle films exhibit both high luminescence efficiency and long-term *** research demonstrates that mobility limitations and anisotropic alignments in CsPbBr3nanocube monolayer films are key to their stabilization, hindering spontaneous growth through face-to-face fusion and resulting in the formation of connecting necks in a diagonal direction. Introducing laser irradiation confirmed this by significantly accelerating nanocubes growth, increasing mobility, and enhancing local structural ordering, leading to larger and more regularly shaped nanosheets. Fourier transform infrared spectroscopy and energy dispersive spectroscopy line-scan analyses indicated that laser irradiation did not disrupt the ligand structure. Transmission electron microscopy and correlative cathodoluminescence electron microscopy revealed the effects of post-growth and heterogeneous structures, including enhanced luminescence and inhomogeneous intensity in the nanosheets. These findings deepen the understanding of the post-growth mechanism of monolayer nanoparticles and the structure-emission correlation and highlight the unique role of laser irradiation in directing the formation of well-defined and regular nanostructures.

关键词： Post-growth mechanism Heterogeneous structure Single-particle spectroscopy Laser irradiation

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Boosting charge extraction and efficiency of inverted perovskite solar cells through coordinating group modification at the buffer layer/cathode interface

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Nano Research 2025年第1期18卷 415-423页

作者： Zhiqing Liang Ziqiu Ren Ziyu Wang Nan Yan Ling Li Bo Zhang Yanlin Song College of Chemistry Zhengzhou UniversityZhengzhou 450052China Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710119China Key Laboratory of Green Printing Institute of ChemistryChinese Academy of Sciences(ICCAS)Beijing Engineering Research Center of Nanomaterials for Green Printing TechnologyNational Laboratory for Molecular Sciences(BNLMS)Beijing 100190China

In inverted perovskite solar cells (PSCs),effective modification of the interface between the metalcathode and electron transport layer (ETL) is crucial forachieving high performance and stability. Herein, sulfonatedbathocuproine, commonly known as disodium bathocuproinedisulfonate (BCDS), was employed as a cathode buffer layerto address the interfacial issues at the [6,6]-phenyl-C61-butyricacid methyl ester (PCBM)/Ag interface. BCDS possesses theability to form coordinate bonds with Ag electrodes. Theutilization of the BCDS buffer layer enhanced the chargeextraction capability at the cathode interface whilesimultaneously achieving interfacial defect passivation,improving interfacial contact and increasing the built-in electricfield. Consequently, a power conversion efficiency (PCE) of25.06% was achieved. Furthermore, owing to the excellent filmforminguniformity of BCDS on PCBM, the stability of thedevice was also improved. After storage in dry air for morethan 2000 h, the device maintained 96% of its initial efficiency. This work underscores the remarkable potential of tailoringcoordination groups to enhance charge extraction efficiency at the ETL-cathode interface, unveiling a promising newfrontier in buffer layer development and performance optimization strategies for PSCs.

关键词： perovskite solar cells buffer layer bathocuproine disulfonate coordination group modification electron transport layer(ETL)-cathode interface

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Theoretical methods for excited state dynamics of molecules and molecular aggregates

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Science China Chemistry 2013年第9期56卷 1271-1276页

作者： SHI Qiang CHEN Hui Beijing National Laboratory for Molecular Science (bnlms) Institute of ChemistryChinese Academy of Sciences

This contribution provides a summary of proposed theoretical and computational studies on excited state dynamics in molecular aggregates, as an important part of the National Natural Science Foundation (NNSF) Major Project entitled "Theoretical study of the low-lying electronic excited state for molecular aggregates". This study will focus on developments of novel methods to simulate excited state dynamics of molecular aggregates, with the aim of understanding several important chemical physics processes, and providing a solid foundation for predicting the opto-electronic properties of organic functional materials and devices. The contents of this study include: (1) The quantum chemical methods for electronic excited state and electronic couplings targeted for dynamics in molecular aggregates; (2) Methods to construct effective Hamiltonian models, and to solve their dynamics using system-bath approaches; (3) Non-adiabatic mixed quantum-classic methods targeted for molecular aggregates; (4) Theoretical studies of charge and energy transfer, and related spectroscopic phenomena in molecular aggregates.

关键词： excited state dynamics molecular aggregates effective Hamiltonian models mixed quantum-classical dynamics

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Reversible self-assembly of gold nanorods mediated by photoswitchable molecular adsorption

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Nano Research 2019年第7期12卷 1563-1569页

作者： Qian Wang Di Li Junyan Xiao Fucheng Guo Limin Qi Beijing National Laboratory for Molecular Sciences (bnlms) College of ChemistryPeking UniversityBeijing 100871China

Stimuli-responsive self-assembly of nanoparticles represents a powerful strategy to achieve reconfigurable materials with novel functionalities and promising *** this regard,light-induced reversible self-assembly (LIRSA) of nanoparticles is most attractive but it is usually limited by the prerequisite yet cumbersome chemical functionalizations of the particle *** we describe an innovative method to realize LIRSA of gold nanorods (GNRs) without surface functionalization through photoswitchable adsorption of an anionic azobenzene derivate *** LIRSA of GNRs is caused by the reversible change between a nearly neutral state and a highly charged state of the GNRs arising from the photoswichable adsorption of AzoNa triggered by *** LIRSA behavior can be readily adjusted by changing the concentration of AzoNa and the aspect ratio of the *** new LIRSA strategy may provide a convenient and efficient route toward light-triggered reversibly reconfigurable nanomaterials.

关键词： self-assembly of nanoparticles gold nanorods reversible self-assembly photoswichable adsorption reconfigurable nanomaterials

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Uptake of isoprene, methacrylic acid and methyl methacrylate into aqueous solutions of sulfuric acid and hydrogen peroxide

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Journal of Environmental Sciences 2012年第11期24卷 1947-1953页

作者： Ze Liu Maofa Ge Weigang Wang Beijing National Laboratory for Molecular Science (bnlms) State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Beijing National Laboratory for Molecular Science (bnlms) Peking University Beijing 100871 China

Multiphase acid-catalyzed oxidation by hydrogen peroxide has been suggested to be a potential route to secondary organic aerosol formation from isoprene and its gas-phase oxidation products, but the lack of kinetics data significantly limited the evaluation of this process in the atmosphere. Here we report the first measurement of the uptake of isoprene, methacrylic acid and methyl methacrylate into aqueous solutions of sulfuric acid and hydrogen peroxide. Isoprene cannot readily partition into the solution because of its high volatility and low solubility, which hinders its further liquid-phase oxidation. Both methacrylic acid and methyl methacrylate can enter the solutions and be oxidized by hydrogen peroxide, and steady-state uptake was observed with the acidity of solution above 30 wt.% and 70 wt.%, respectively. The steady-state uptake coefficient of methacrylic acid is much larger than that of methyl methacrylate for a solution with same acidity. These observations can be explained by the different reactivity of these two compounds caused by the different electron-withdrawing conjugation between carboxyl and ester groups. The atmospheric lifetimes were estimated based on the calculated steady-state uptake coefficients. These results demonstrate that the multiphase acid-catalyzed oxidation of methacrylic acid plays a role in secondary organic aerosol formation, but for isoprene and methyl methacrylate, this process is not important in the troposphere.

关键词： multiphase acid-catalyzed oxidation uptake steady-state uptake coefficient secondary organic aerosol

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Heterogeneous uptake of nitrogen dioxide on Chinese mineral dust

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Journal of Environmental Sciences 2015年第12期27卷 110-118页

作者： Li Zhou Weigang Wang Siqi Hou Shengrui Tong Maofa Ge Beijing National Laboratory for Molecular Science (bnlms) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of Sciences Beijing National Laboratory for Molecular Science (bnlms) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesPeking University

Mineral dust is one of the major aerosols in the *** assess its impact on trace atmospheric gases,in this work we present a laboratory study of the effect of temperature on the heterogeneous reaction of NO2 on the surface of ambient Chinese dust over the temperature range from 258 to 313 *** results suggest that nitrogen dioxide could mainly be adsorbed on these types of Chinese mineral dust reversibly with little temperature *** to a previous study on NO2 uptake on mineral aerosols,the uptake coefficients are mainly on the order of 10^（-6） for the Chinese dust,when BET areas are taken into *** was observed as a product,and its formation and decomposition on Chinese mineral dust during the uptake processes were also *** complete dataset from this study was compiled with previous literature *** implications of the heterogeneous reaction between NO2 and mineral dust are also discussed,in an effort to understand this important heterogeneous process.

关键词： Mineral dust Nitrogen dioxide Uptake coefficient Temperature dependence

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Knudsen cell and smog chamber study of the heterogeneous uptake of sulfur dioxide on Chinese mineral dust

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Journal of Environmental Sciences 2014年第12期26卷 2423-2433页

作者： Li Zhou Weigang Wang Yanbo Gai Maofa Ge Beijing National Laboratory for Molecular Science (bnlms) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of Chemistry Chinese Academy of Sciences Beijing National Laboratory for Molecular Science (bnlms) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesPeking University

The heterogeneous uptake processes of sulfur dioxide on two types of Chinese mineral dust（Inner Mongolia desert dust and Xinjiang sierozem） were investigated using both Knudsen cell and smog chamber system. The temperature dependence of the uptake coefficients was studied over a range from 253 to 313 K using the Knudsen cell reactor, the initial uptake coefficients decreased with the increasing of temperature for these two mineral dust samples, whereas the steady state uptake coefficients of the Xinjiang sierozem increased with the temperature increasing, and these temperature dependence functions were obtained for the first time. In the smog chamber experiments at room temperature, the steady state uptake coefficients of SO2 decreased evidently with the increasing of sulfur dioxide initial concentration from 1.72 × 1012 to 6.15 × 1012mol/cm3. Humid air had effect on the steady state uptake coefficients of SO2 onto Inner Mongolia desert *** about the understanding of the uptake processes onto mineral dust samples and the environmental implication were also discussed.

关键词： Mineral dust Sulfur dioxide Uptake coefficient Temperature dependence

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A Miniature Droplet Reactor Built on Nanoparticle-Derived Superhydrophobic Pedestals

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Nano Research 2011年第3期4卷 266-273页

作者： Bin Su, Shutao Wang Yanlin Song Lei Jiang Beijing National Laboratory for Molecular Science （bnlms） Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

The capability to design and modulate materials, shapes, heat transfer, and mass mixing during the process of developing chemical reactors has allowed researchers to explore millions of chemical reactions and assays. However, despite the advantages in engineering array-based microreactors or microfluidic systems, the wetting attachment between solutions of reagents/products and the glass or polymer substrates of containers leads to difficulties in collecting products effectively and preventing channel blockage. Herein we present a miniature droplet reactor which takes advantage of the anti-wetting and low-adhesive properties of nanoparticle-derived superhydrophobic pedestals, allowing aqueous droplets to be manipulated freely but also providing a confined environment for performing a series of aqueous phase chemical reactions on a small scale. Gas- or precipitate- forming reactions can also be performed inside this miniature reactor. Most importantly, reaction products in liquid, solid or gaseous states can be collected effectively, which allows the harvesting of valuable products formed in limited amounts. Such a miniature reactor built on superhydrophobic pedestals provides a new way of performing common chemical reactions and may open the door to the design of next-generation microreaction systems.

关键词： Superhydrophobic reactor droplet hybrid materials nanomaterials

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Synthesis and dehydrogenation properties of NaZn(BH4)3·en and NaZn(BH4)3·2en(en= ethylene diamine)

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Journal of Energy Chemistry 2020年第3期29卷 233-236页

作者： Yong Wu Yue Qi Jie Zheng Xingguo Li Beijing National Laboratory for Molecular Sciences(bnlms) College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Two new hydrogen storage compounds,Na Zn(BH4)3·en and Na Zn(BH4)3·2en(en=ethylene diamine)are synthesized by a solution *** can release 6.4 wt%and 6.3 wt%pure hydrogen below 200℃,respectively,demonstrating the potential to be used as hydrogen ***,their dehydrogenation products,thermodynamics and kinetics are well characterized and *** shows that the stronger Zn-N interactions and the Hδ+–Hδ-interactions are significant for their stability below 100℃,relatively low decomposition temperatures and elimination of gas impurities.

关键词： Borohydride Ethylene diamine Hydrogen storage

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Phase Behavior of Amphiphiles at Liquid Crystals/Water Interface: A Coarse-grained Molecular Dynamics Study

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Chinese Journal of Polymer Science 2014年第10期32卷 1298-1310页

作者： Yu-ting Ouyang 郭洪霞 Beijing National Laboratory for Molecular Sciences (bnlms) State Key Laboratory for Polymer Physics and ChemistryInstitute of Chemistry Chinese Academy of Sciences

We present a coarse-grained molecular dynamics simulation study of phase behavior of amphiphilic monolayers at the liquid crystal （LC）/water interface. The results revealed that LCs at interface can influence the lateral ordering of amphiphiles. Particularly, the amphiphile tails along with perpendicularly penetrated LCs between tails undergo a two-dimension phase transition from liquid-expanded into a liquid-condensed phase as their area density at interface reaches 0.93. While, the liquid-condensed phase of the monolayer never appears at oil/water interface with isotropic shape oil particles. These findings reveal the penetration of anisotropic LC can promote ordered lateral organization of amphiphiles. Moreover, we find the phase transition point is shifted to lower surface coverage of amphiphiles when the LCs have larger affinity to the amphiphile tails.

关键词： Phase behavior Amphiphilic monolayer Lateral ordering Molecular simulation Liquid crystal.

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