Bio-inspired catalyst materials with diverse functions and excellent performance are highly demanded for efficient catalytic conversion.However,precisely imitating the natural structures to achieve optimized performan...Bio-inspired catalyst materials with diverse functions and excellent performance are highly demanded for efficient catalytic conversion.However,precisely imitating the natural structures to achieve optimized performance is still highly challenging.Inspired by the fast mass diffusion and exchange ability of alveolus structures,we prepared a hierarchically macro-meso-microporous TS-1 zeolite microsphere with a precisely designed alveolus-like structure(HAS-TS-1)by developing a method that combined template and emulsion approaches.These alveolus-like zeolite microspheres possessed interconnected macropores(280 nm)and mesopores(40 nm),with a BET surface area of 484 m^(2) g^(-1).This novel bio-inspired structure showed a significantly enhanced adsorption ability for thiophenic molecules,which was four times greater than that exhibited by a microporous TS-1 zeolite.HAS-TS-1 exhibited excellent catalytic oxidative desulfurization performance of a series of bulky thiophenic molecules,completely removing 4,6-dimethyldibenzothiophene(DMDBT)in 15 min,which was twelve times faster than that observed using a TS-1 microsphere(180 min).The superiority of this bio-inspired hierarchically alveolus-like structure in mass transfer and diffusion may enable its advanced application in the fields of catalysis,energy,and sensors.展开更多
The aggregation process plays a significant role in regulating the aggregate structures from molecules toward macroscopic photophysical properties.Pyrene(Py),as the simplest dimer candidate,serves as a suitable model ...The aggregation process plays a significant role in regulating the aggregate structures from molecules toward macroscopic photophysical properties.Pyrene(Py),as the simplest dimer candidate,serves as a suitable model for studying the aggregation.Herein,a series of Py-based aggregation-induced emission(AIE)materials have been investigated by clarifying the comprehensive roles of oxygen,substituents,molecular motion,and packing during aggregation,initially realizing the aim of controlling aggregate structures.With a largely planar and conjugated conformation,Py shows anomalous AIE characteristics due to the oxygen quenching at the molecular level but turn-on fluorescence in the aggregate state because of the oxygen isolation.Although introducing substituents induces molecular motion and similarly weakened luminescence in the molecular state,the impact of substituents on the aggregate-state photophysical properties enormously differs,exhibiting from weak blue,strong cyan,and strong green to weak yellow emissions,due to variable aggregate structures.Interestingly,the natural alicycle-substituted Py-dehydroabietylamine(Py-DAA)exhibits both mechanochromism and acidichromism,which can be synergistically applied in dynamic encryption-decryption.This work not only elucidates the unique AIE property of Py for the first time but also clarifies the bridging role of aggregation between single-molecular and aggregate states,achieving preliminary control over the aggregate structures.展开更多
基金financially supported by the National Key R&D Program of China(2022YFB3504000)National Natural Science Foundation of China(22293022,U22B6011,22402155)+5 种基金Program of Introducing Talents of Discipline to Universities-Plan 111(Grant No.B20002)from the Ministry of ScienceTechnology and the Ministry of Education of China,Postdoctoral Fellowship Program of CPSF(GZC20232012,2023M742724)L.H.Chen acknowledges Hubei Provincial Department of Education for the“Chutian Scholar”programB.L.Su acknowledges the Clare Hall Life Membership,University of CambridgeThis research was also supported by the European Commission Interreg V France-Wallonie-Vlaanderen project“DepollutAir”,the Program Win2Wal(TCHARBONACTIF:2110120)Wallonia Region of Belgium and the National Key R&D Program Intergovernmental Technological Innovation Special Cooperation Project Wallonia-Brussels/China(MOST)(SUB/2021/IND493971/524448).
文摘Bio-inspired catalyst materials with diverse functions and excellent performance are highly demanded for efficient catalytic conversion.However,precisely imitating the natural structures to achieve optimized performance is still highly challenging.Inspired by the fast mass diffusion and exchange ability of alveolus structures,we prepared a hierarchically macro-meso-microporous TS-1 zeolite microsphere with a precisely designed alveolus-like structure(HAS-TS-1)by developing a method that combined template and emulsion approaches.These alveolus-like zeolite microspheres possessed interconnected macropores(280 nm)and mesopores(40 nm),with a BET surface area of 484 m^(2) g^(-1).This novel bio-inspired structure showed a significantly enhanced adsorption ability for thiophenic molecules,which was four times greater than that exhibited by a microporous TS-1 zeolite.HAS-TS-1 exhibited excellent catalytic oxidative desulfurization performance of a series of bulky thiophenic molecules,completely removing 4,6-dimethyldibenzothiophene(DMDBT)in 15 min,which was twelve times faster than that observed using a TS-1 microsphere(180 min).The superiority of this bio-inspired hierarchically alveolus-like structure in mass transfer and diffusion may enable its advanced application in the fields of catalysis,energy,and sensors.
基金supported by the National Natural Science Foundation of China(21601087)the Natural Science Foundation of Jiangsu Province(BK20231296)+3 种基金the Open Fund of Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates,Guangzhou 510640,China(South China University of Technology[2023B1212060003])the Shenzhen Key Laboratory of Functional Aggregate Materials(ZDSYS20211021111400001)the Science Technology Innovation Commission of Shenzhen Municipality(KQTD20210811090142053)the Key Research and Development Project of Yunnan Province(202303AC100010).
文摘The aggregation process plays a significant role in regulating the aggregate structures from molecules toward macroscopic photophysical properties.Pyrene(Py),as the simplest dimer candidate,serves as a suitable model for studying the aggregation.Herein,a series of Py-based aggregation-induced emission(AIE)materials have been investigated by clarifying the comprehensive roles of oxygen,substituents,molecular motion,and packing during aggregation,initially realizing the aim of controlling aggregate structures.With a largely planar and conjugated conformation,Py shows anomalous AIE characteristics due to the oxygen quenching at the molecular level but turn-on fluorescence in the aggregate state because of the oxygen isolation.Although introducing substituents induces molecular motion and similarly weakened luminescence in the molecular state,the impact of substituents on the aggregate-state photophysical properties enormously differs,exhibiting from weak blue,strong cyan,and strong green to weak yellow emissions,due to variable aggregate structures.Interestingly,the natural alicycle-substituted Py-dehydroabietylamine(Py-DAA)exhibits both mechanochromism and acidichromism,which can be synergistically applied in dynamic encryption-decryption.This work not only elucidates the unique AIE property of Py for the first time but also clarifies the bridging role of aggregation between single-molecular and aggregate states,achieving preliminary control over the aggregate structures.
