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Rational design of ZnCdS/TpPa-1-COF heterostructure photocatalyst by strengthening the interface connection in solar hydrogen production reactions

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Nano Research 2024年第3期17卷 1027-1034页

作者： Di Yang Zhi-Gang Li Xinghao Zhang Zenghuan Ren Weihan Lu Haining Liu Xiaomeng Guo Jijie Zhang Xian-He Bu tianjin key laboratory of metal and molecule-based material chemistry School of Materials Science and EngineeringNankai UniversityTianjin 300350China College of chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China State key laboratory of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

ZnCdS quantum dots(QDs)are highly coveted in photocatalysis research for their exceptional visible-light responses and high light-absorption ***,their practical application is hindered by their tendency to aggregate,due to having high surface *** address this issue,herein,a heterostructure is synthesized by growing ZnCdS QDs with a size of approximately 5 nm onto the surface of a two-dimensional(2D)covalent organic framework(COF),*** approach suppresses the aggregation of the QDs and improves their *** ZnCdS/TpPa-1-COF composite exhibited a peak hydrogen evolution rate of 6244.16μmol·g^(-1)·h^(-1),which was 2.89 and 4.18 times greater than that of ZnCdS and TpPa-1-COF,*** zero-dimensional/two-dimensional(0D/2D)heterojunction formed by ZnCdS and TpPa-1-COF generates a strong interfacial force,which is attributed to the intimate contact between the *** connections accelerate charge separation,improve the utilisation of reduced electrons,and reduce the extent of agglomeration of the ZnCdS QDs,thereby resulting in high hydrogen production activity of the ***,the photocatalytic mechanism is studied using Kelvin probe force microscopy and theoretical *** study offers a novel approach for creating sulfide photocatalysts and is crucial for investigating the potential practical applications of the related photocatalysts.

关键词： covalent organic frameworks quantum dots photocatalysis hydrogen generation heterojunction

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Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting

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Nano Research 2024年第3期17卷 1114-1122页

作者： Chao-Peng Wang Hao Sun Gang Bian Jia-Xi Wang Xixi Pang Guoqi Wang Jian Zhu Xian-He Bu School of materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China tianjin key laboratory of metal and molecule-based material chemistry Nankai UniversityTianjin 300350China tianjin key laboratory for Rare Earth materials and Applications Nankai UniversityTianjin 300350China

Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient ***,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)*** particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 ***,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V *** study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.

关键词： layer-by-layer(LbL)assembly layered double hydroxides(LDH) two-dimensional(2D)electrocatalysts oxygen evolution reaction(OER) water splitting

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Enhancing Low-Frequency Microwave Absorption Through Structural Polarization Modulation of MXenes

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Nano-Micro Letters 2024年第10期16卷 435-452页

作者： Bo Shan Yang Wang Xinyi Ji Yi Huang College of Light Industry Science and Engineering State Key Laboratory of Biobased Fiber Manufacturing TechnologyTianjin University of Science and TechnologyTianjin 300457People's Republic of China National Institute for Advanced materials Tianjin Key Laboratory of Metal and Molecule Based Material ChemistryKey Laboratory of Functional Polymer MaterialsCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)School of Materials Science and EngineeringNankai UniversityTianjin 300350People's Republic of China

Two-dimensional carbon-based materials have shown promising electromagnetic wave absorption capabilities in mid-and high-frequency ranges,but face challenges in low-frequency absorption due to limited control over polarization response mecha-nisms and ambiguous resonance *** this study,we pro-pose a novel approach to enhance absorption efficiency in aligned three-dimensional(3D)MXene/CNF(cellulose nanofibers)cavities by modifying polarization properties and manipulating resonance response in the 3D MXene *** controlled polarization mechanism results in a significant shift of the main absorption region from the X-band to the S-band,leading to a remarkable reflection loss value of-47.9 dB in the low-frequency ***,our findings revealed the importance of the oriented electromagnetic coupling in influencing electromagnetic response and microwave absorption *** present study inspired us to develop a generic strategy for low-frequency tuned absorption in the absence of magnetic element participation,while orientation-induced polarization and the derived magnetic resonance coupling are the key controlling factors of the method.

关键词： Hierarchical structure MXene Microwave absorption Low-frequency

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Construction of a Cu@hollow TS-1 nanoreactor based on a hierarchical full-spectrum solar light utilization strategy for photothermal synergistic artificial photosynthesis

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Carbon Energy 2024年第2期6卷 25-36页

作者： Sixian Zhu Qiao Zhao Hongxia Guo Li Liu Xiao Wang Xiwei Qi Xianguang Meng Wenquan Cui Hebei key laboratory for Environment Photocatalytic and Electrocatalytic materials College of Chemical EngineeringNorth China University of Science and TechnologyTangshanChina School of materials Science and Engineering National Institute for Advanced MaterialsTKL of Metal and Molecule-Based Material ChemistryNankai UniversityTianjinChina Hebei Iron and Steel laboratory TangshanChina

The artificial photosynthesis technology has been recognized as a promising solution for CO_(2) *** catalysis has been proposed as a novel strategy to promote the efficiency of artificial photosynthesis by coupling both photochemistry and ***,strategies for maximizing the use of solar spectra with different frequencies in photothermal catalysis are urgently ***,a hierarchical full-spectrum solar light utilization strategy is *** on this strategy,a Cu@hollow titanium silicalite-1 zeolite(TS-1)nanoreactor with spatially separated photo/thermal catalytic sites is designed to realize high-efficiency photothermal catalytic artificial *** space-time yield of alcohol products over the optimal catalyst reached 64.4μmol g−1 h−1,with the selectivity of CH3CH2OH of 69.5%.This rationally designed hierarchical utilization strategy for solar light can be summarized as follows:(1)high-energy ultraviolet light is utilized to drive the initial and difficult CO_(2) activation step on the TS-1 shell;(2)visible light can induce the localized surface plasmon resonance effect on plasmonic Cu to generate hot electrons for H2O dissociation and subsequent reaction steps;and(3)low-energy near-infrared light is converted into heat by the simulated greenhouse effect by cavities to accelerate the carrier *** work provides some scientific and experimental bases for research on novel,highly efficient photothermal catalysts for artificial photosynthesis.

关键词： artificial photosynthesis full spectrum nanoreactors photothermal catalysis

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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao key laboratory of Advanced Energy material chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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Energy transfer, anticounterfeiting, white light emission and sensing in fine-regulating series of lanthanide metal-organic frameworks

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Journal of Rare Earths 2024年第3期42卷 446-454,I0001页

作者： Juanjuan Xue Yao Wang Guoping Yang Yaoyu Wang key laboratory of Synthetic and Natural Functional molecule chemistry of the Ministry of Education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry&Materials ScienceNorthwest UniversityXi'an710127China

Three lanthanide ions and a rigid(1,1'-biphenyl)-2,4,6-tricarboxylic acid(H_(3)bptc) ligand led to the isostructural lanthanide metal-organic frameworks(Ln-MOFs) {[Ln(bptc)(H_(2)O)_(3)]·3H_(2)O}_n(Lnbptc, Ln = Eu,Tb, Gd, Eu_(x)Tb_(1—x), Eu_(x)Gd_(1-x), Tb_(x)Gd_(1-x), and Eu_(0.12)Tb_(0.52)Gd_(0.36)). The density functional theory(DFT) and time-dependent DFT calculation were expanded on H_3bptc, which point to the occurrence of “antenna effect”. The minor diameter samples of Eubptc, Tbbptc, and Gdbptc can also be attained via the microwave synthesis and employed for handwriting anticounterfeiting. Interestingly, the typical red emission of Eu^(3+) and green emission of Tb~(3+) could be fine-tuned by Gd^(3+) via chemical mixing to be full-color emissions bimetallic doped Eu_(x)Tb_(1-x)bptc, Eu_(x)Gd_(1-x)bptc, and Tb_(x)Gd_(1-x)bptc. The above synthetic bimetallic MOFs can be fixed in positioning boxes of quick response(QR) codes with diverse emission for anticounterfeiting. The message can be decoded under the irradiation of 365 nm ultraviolet lamp while invisible in the daylight. Notably, the trimetallic doped Eu_(0.12)Tb_(0.52)Gd_(0.36)bptc emits white light with the CIE color coordinate(0.34, 0.34). Furthermore, Tbbptc is demonstrated to be a sensitive probe toward nitrobenzene and acetone with multiple mechanisms.

关键词： metal-organic frameworks Anticounterfeiting White light-emitting Sensing Rare earths

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NHC-derived carbon-centered luminescent radicals with shortwavelength emission via suppression of Kasha's rule

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Science China chemistry 2024年第8期67卷 2679-2685页

作者： Can Chen Xin Li Xinhua Ouyang Ying-Feng Han key laboratory of Synthetic and Natural Functional molecule chemistry of the Ministry of Education Xi’an Key Laboratory of Functional Supramolecular Structure and MaterialsCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an 710127China College of material Engineering Fujian Agriculture and Forestry University Fuzhou 350108China

Luminescent organic radicals have garnered increasing attention owing to their versatile applications in sensing, imaging, and organic light-emitting diodes(OLEDs), attributed to their unique emission properties originating from the doublet spin ***, the natural narrow bandgap of organic free radicals typically limits their emission to the long-wavelength *** luminescent organic radicals with short-wavelength emission remains a significant challenge. Herein, a series of carbon-centered radicals with short-wavelength emission(383–476 nm) by combining N-heterocyclic carbenes with various polycyclic aromatic hydrocarbons(PAHs)(2-naphthyl, 2a~Ⅰ and 2b~Ⅰ;2-phenanthryl, 2a~Ⅱand 2b~Ⅱ;2-anthryl, 2a~Ⅲand 2b~Ⅲ;3-phenanthryl, 2a~Ⅳand 2b~Ⅳ). Theoretical calculations reveal that the introduction of PAHs significantly increases the ΔE_(D2-D1) in 2a^(Ⅰ–Ⅲ)and 2b^(Ⅰ–Ⅲ)compared to that in phenyl-derived radical congeners. Consequently, the internal transition from D2 to D1 is impeded, leading to a high yield of D2 emission and a suppressed Kasha's rule, thereby overcoming the limitations imposed by their narrow bandgap. For 2a~Ⅳ and 2b~Ⅳ, despite a moderately large ΔED2-D1value, the ΔED3-D1value exceeds 1 e V, indicating that their emission likely originates from the D3 state. Furthermore, we utilized 2a~Ⅲand 2b~Ⅲ as emissive materials in OLEDs,resulting in blue emissions with external quantum efficiencies of 7.5% and 6.5%, respectively.

关键词： N-heterocyclic carbenes luminescent organic molecules carbon-centered radicals short-wavelength emission

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Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5179-5187页

作者： Jinlei Qin Rui Wang Zilong Yuan Pei Xiao Deli Wang key laboratory of material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low ***,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper t... 详细信息

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox

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Porous organic cages as a novel platform for second harmonic generation

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Science China chemistry 2024年

作者： Feng Shui Yunqin Zhang Mao Yi Xiongli Liu Lin Li Shuo Zhang Yongshen Zheng Yongtao Yao Qiao Zhao Baiyan Li Xianhe Bu School of materials Science and Engineering National Institute for Advanced Materials TKL of Metal and Molecule-Based Material Chemistry Nankai University National key laboratory of Science and Technology on Advanced Composites in Special Environments Harbin Institute of Technology

Second harmonic generation(SHG) is one of the most extensively applied nonlinear optical phenomena. Compared to traditional inorganic SHG materials, organic SHG materials, including non-centrosymmetric small molecular crystals and organic polymers, have been extensively explored for SHG optics due to their advantageous properties, including high light-induced damage threshold, ultrafast response speed, high polarization ratio, wide transparency range, and elevated dielectric constant. However,in organic SHG materials, most small molecular crystals often show poor thermal stability(material with high thermal stability, large-size crystals,excellent processability, high homogeneity, and a well SHG effect. In the contribution, we developed herein porous organic cages(POCs) as a novel platform for SHG optics. Thanks to its inherent macromolecular composition and zero-dimensional discrete structures, POCs can not only solve the instability problem of small molecule crystals but also overcome the drawbacks in growing large-size crystals for organic polymer. The obtained two POCs with chiral asymmetric centers(CPOC-R-5 and CPOCS-7) display advantageous features for SHG optics including well SHG performance, large-size crystal(5 mm×3 mm×1 mm),high thermal stability(≥250 °C), wide transparency window(750–2,000 nm) and high polarization ratio(up to 94.5%). This work thus develops POCs as a new platform toward the construction of organic NLO materials with the potential application in sorts of SHG optics.

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Dual polarization strategy to enhance CH_(4) uptake in covalent organic frameworks for coal-bed methane purification

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Chinese Chemical Letters 2024年第8期35卷 545-548页

作者： Junhua Wang Xin Lian Xichuan Cao Qiao Zhao Baiyan Li Xian-He Bu School of materials Science and Physics China University of Mining and TechnologyXuzhou 221116China School of Chemical Engineering and Technology China University of Mining and TechnologyXuzhou 221116China School of materials Science and Engineering National Institute for Advanced MaterialsTKL of Metal and Molecule-Based Material ChemistryNankai UniversityTianjin 300350China

The purification of low-grade coal-bed methane is extremely important,but challenging,due to the very similar physical properties of CH_(4)and ***,we proposed a dual polarization strategy by employing triazine and polyfluoride sites to construct polar pores in COF materials,achieving the efficient separa-tion of CH_(4)from *** expected,the dual polarized F-CTF-1 and F-CTF-2 exhibit higher CH_(4)adsorption capacity and CH_(4)/N_(2)selectivity than CTF-1 and CTF-2,***,the CH4 uptake capacity and CH_(4)/N_(2)selectivity of F-CTF-2 is 1.76 and 1.42 times than that of *** work not only developed promising COF materials for CH4/N_(2)separation,but also provided important guidance for the separation of other adsorbates with similar properties.

关键词： Dual polarization strategy Covalent organic frameworks(COFs) Coal-bed methane purification Chemical/thermal stability Cycling stability

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