Materials Chemistry Frontiers
·
2022
·Vol. 7
·期 4
·705-712
·
IF 8.683
Jiantao Yuan,Guojun Zhou,Jian Zhang,Xian-Ming Zhang
Although low-dimensional hybrid metal halides have recently been the subject of considerable attention as white-light emitters, the superiority of structural diversity has not been relied upon to tune photoluminescence (PL) behaviors by synergistic control of organic and inorganic compositions. Herein, a series of distinctive cadmium halides (C6H7NX)2CdX4 (X = Cl, Br, I) with π-conjugated ligands and halogen substitution are developed, in which the isolated [CdX4]2− tetrahedrons are separated by large [C6H7NX]+ organic cations into a unique zero-dimensional (0D) host-guest structure. Intriguingly, the synergetic controlling of π-conjugated ligands and [CdX4]2− units enables single-component ultra-broadband white-light emissions with a record color rendering index (CRI) of 99 in the above novel 0D cadmium halides. (C6H7NCl)2CdCl4 and (C6H7NBr)2CdBr4 exhibit ultra-broadband cold white-light emission with large full-width at half-maximum (FWHM) of 218 nm and 244 nm, respectively, which is triggered by the synergistic emissions of [C6H7NX]+ ligands and self-trapped excitons (STEs) of Cd2+. A comparison of PL properties of cadmium halides with Cl/Br/I transmutation elucidated that the nature of the halogens is strongly dependent on the trapping/de-trapping of STEs as well as on the π → π* transition of the π-conjugated ligands, along with the resulting PL modulation on emission intensities, wavelengths, and FWHM. This work reveals a unique synergetic model for implementing white-light emission and extends to the design of high-performance hybrid emitters.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Man Dong,Qingqing Pan,Fanfei Meng,Xiaohui Yao,Siqi You,Guogang Shan,Chunyi Sun,Xinlong Wang,Zhongmin Su
Sunlight-driven CO 2 reduction to value-added chemicals is an effective strategy to promote carbon recycling. The exploration of catalysts with efficient charge separation is crucially important for highly efficient CO 2 photoreduction. In this work, the preparation of metal-cluster-based covalent organic framework (CuABD) integrated features from both metal organic frameworks (MOFs) and covalent organic frameworks (COFs) through the condensation of diamines and functionalized trinuclear copper clusters demonstrate a thoughtful design strategy. The reported yield of 1.3 mmol g −1 h −1 for formic acid (HCOOH) under simulated solar irradiation is impressive, surpassing the performance of many COF- and MOF-based catalysts previously reported. Compared to its isomorphic metal-free structure (named BDFTD) and bare trinuclear Cu cluster which present extremely poor catalytic activities, CuABD displays remarkably enhanced CO 2 reduction activity. Experimental and theoretical investigations reveal that the efficient charge transfer between diamine monomer and cyclic trinuclear copper (I) units, and the electron delocalization of the π-conjugated framework are responsible for the appealing catalytic performance. In summary, the work presents a well-structured and scientifically sound exploration of a metal-cluster-based covalent organic framework for efficient CO 2 reduction under sunlight.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2016
·Vol. 20
·期 8
·2169-2177
·
IF 2.327
Zhang Tao,Li Han,Tang Qianqiu,Sun Minqiang,Wang Gengchao
Organic compounds become promising candidates for cathodes of rechargeable lithium battery (RLB) due to the high theoretical capacity and improved safety. However, they exhibit low conductivity and easy dissolution in electrolyte, which leads to the low utilization of active materials and poor cycling stability of RLBs. Here, we synthesize a novel composite of activated hierarchical porous carbon supporting poly(1,5-diamino-anthraquinone) ( a HPC@PDAA), using Ce(SO 4 ) 2 as oxidant and naphthalenesulfonic acid (NSA) as soft template for PDAA. The as-synthesized composite exhibits uniformly nanoporous structure with nano-sized PDAA particles distributed homogenously inside and outside of pores. The a HPC@PDAA cathode for RLBs achieves high electrochemical performance with a discharge capacity as much as 250 mAh g −1 at the current density of 100 mA g −1 , which still maintains 176 mAh g −1 after 2000 charging-discharging cycles.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 11
·期 1
·107-113
·
IF 7
Zihao Yu,Qingran Ding,Yuhang Jiang,Weiqi Huang,Changsheng Yang,Sangen Zhao,Junhua Luo
The research on nonlinear optical (NLO) crystals is mainly focused on two relatively separate systems, π-conjugated or non-π-conjugated systems, respectively. In this work, we report a new NLO crystal Na10Zn(NO3)4(SO3S)4 combining inorganic π-conjugated [NO3] and non-π-conjugated heteroanion [S2O3] groups, which was synthesized by the aqueous solution method. In the structure, the similar coexistence of planar triangular anionic groups (π-conjugated) and heteroanion tetrahedra (non-π-conjugated) is rarely mentioned, which provides a new approach for designing NLO crystals. Notably, this compound exhibits a phase-matching second-harmonic generation (SHG) response 1.2 times that of KH2PO4. In addition, birefringence, absorption edge and theoretical calculations are also reported in this article. This work provides a new designing route to expand NLO systems via combining planar π-conjugated and non-π-conjugated heteroanion groups.
研究领域:
材料科学
·
光学材料
·
晶体化学
·
非线性光学
·
功能材料
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Yunqi Zhao,Yipeng Song,Yanqiang Li,Wei Liu,Yang Zhou,Weiqi Huang,Junhua Luo,Sangen Zhao,Belal Ahmed
Birefringence is an important linear optical property of anisotropic crystals that plays a significant role in regulating light polarization. A new bialkali–rare earth metal sulfate, NaRbY2(SO4)4 compound, consisting of non-π-conjugated alkali metals and rare earth metal-centered dodecahedral YO8 has been synthesized. The structure analysis suggests that the three-dimensional (3D) structure of the compound is found to be attributable to the combination of dodecahedral YO8 and tetrahedral SO4 groups with Na+ and Rb+ located in the cavities. The ultraviolet, visible, and near-infrared (UV–vis–NIR) spectra reveal that the compound exhibits transparency at a wavelength of less than 200 nm. The observed birefringence of the compound is 0.045@550 nm, which is comparatively larger than that of most deep-ultraviolet (DUV) birefringent crystals. The birefringence mainly originated from the YO8 dodecahedron, which is suggested by first-principles calculations. This research work can provide a useful perspective to explore new DUV sulfates with excellent birefringence.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
Advanced Optical Materials
·
2024
·
IF 8
Muhammad Arif,Xu Liu,Zijian Li,Hangwei Jia,Yansheng Jiang,Zhihua Yang,Xueling Hou,Shilie Pan
Salts and co-crystals composed of planar π -conjugated functional units represent a fascinating class of materials, featuring both enlarged birefringence and a strong SHG effect. Herein, the optical properties of π -conjugated (C 4 H 7 N 3 ) 2+ functional unit within 2-aminopyrimidine (2-AP) family are investigated for the first time. Furthermore, twelve novel compounds are successfully synthesized by applying four different strategies. In these strategies, (C 4 H 7 N 3 ) 2+ , (C 4 H 6 N 3 ) + , and (C 4 H 5 N 3 ) functional units are introduced into the crystal structure, both solely and in combination, to analyze the alteration in birefringence. Remarkably, a birefringence rule with (C 4 H 7 N 3 ) 2+ < (C 4 H 6 N 3 ) + < (C 4 H 5 N 3 ), stating that an increase in net charge over π -conjugated functional unit leads to a reduced birefringence, is discovered. Consequently, the inclusion of a charge-neutral (C 4 H 5 N 3 ) functional unit within the crystal structure along with coplanar arrangement is a promising approach to enhance birefringence. Furthermore, D-2 [(C 4 H 5 N 3 )(H 3 C 3 N 3 O 3 )] realizes Δn calc = 0.412 maximum in the (2-AP) family. Notably, both A-1 [(C 4 H 7 N 3 )(CF 3 SO 3 ) 2 ] and B-1 [(C 4 H 6 N 3 ) 2 (IO 3 ) 2 (H 2 O)] crystalize in the non-centrosymmetric space groups, with B-1 exhibiting SHG efficiency of ≈1.4 × KDP @ 1064 nm, with the shortest λ PM at 384 nm. This work provides new insight into discovering novel birefringent and non-linear optical materials with high performances in the wide chemical space.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULES
·
2024
·
IF 5.1
Guoming Yuan,Hui Yang,Xiaole Zheng,Kunxin Wang,Zhijun Liu,Yuemiao Zhang,Yanhan Tao,Kun Wu,Peiwei Hong,Jun Shi,Li Yang
In response to the limitations imposed on the microelectronics industry by electronic crosstalk losses and signal delays, as well as the rapid accumulation of heat, intrinsically low dielectric and high thermal conductivity materials are in urgent demand. Here, a self-curable biobased silane precursor (M@KH590) with a biphenyl unit was synthesized. A series of films (magnolol polysiloxane films (MPSOs)) were prepared using simple sol–gel film conversion and annealing and modulated intermolecular forces and molecular structure. The red-shift of the UV–vis absorption indicated that a larger π–π conjugated system was established. As a result, the through-plane thermal conductivity of MPSO-140 was 0.601 W·m–1·K–1, which was more than three times that of the pure polysiloxane material. Meanwhile, MPSO-140 exhibited excellent intrinsic low dielectric properties (Dk = 2.52, Df = 0.000572, and f = 100 MHz). This was mainly attributed to the reduction of highly polar substances and groups as well as the difficulty in polarizing a π–π conjugated system. Based on rigid biphenyl units and high cross-link density, the tensile strength and modulus of MPSO-140 were 17.42 MPa and 2.61 GPa, respectively, showing prominent mechanical properties. In addition, MPSO-140 exhibited excellent water resistance (water contact angle and 72 h water absorption of 104.8° and 0.19%, respectively) and electrical insulation, showing great potential for practical applications. The study broadened the way toward overcoming the contradiction between low dielectric and high thermal conductivity by simultaneously introducing large free volume and modulating the intermolecular forces and molecular structure in a simple and effective way.
研究领域:
材料科学
·
电子工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yahui Zhu,Xiaohua Ma,Wenjie Lai,Zengxiang Tang,Weiming Xiao,Rong Zeng,Shunmin Ding,Chao Chen
D-π conjugated coordination polymers (CCPs) are often widely used in photocatalysis and electrocatalysis due to their unique electronic conductivity and structural flexibility. However, it remains a challenge to overcome the self-degradation of d-π CCPs in thermal catalysis and to effectively utilize their excellent electron transfer properties. Here, we present a series of d-π CCPs derivative after calcination treatment. The derivatives were optimized for overall electron cloud density by constructing two-dimensional pyridinic-nitrogen (N) doped carbon carriers, which exhibited the inherent π-electron delocalization and charge transfer properties of d-π CCPs. The presence of electron transfer was confirmed by X-ray Photoelectron Spectroscopy (XPS), Raman and kinetic analysis, demonstrating that this d-π CCPs derivative possesses excellent electron conduction ability and low activation energies for the reaction. Density-functional theory (DFT) calculations further confirmed the modulation of the nickel nanoparticles (Ni NPs) electronic state by the carriers, which resulted in strong Ni NPs interactions with the high-electron-density π-bonds of the C C bond. This property significantly enhances the target adsorption and activation of the C C bond, leading to a substantial enhancement of the reaction performance. This strategy provides a new development direction for the application of d-π CCPs in thermal catalysis.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Zhuo Zhiqiang,Ni Mingjian,Yu Ningning,Zheng Yingying,Lin Yingru,Yang Jing,Sun Lili,Wang Lizhi,Bai Lubing,Chen Wenyu,Xu Man,Huo Fengwei,Lin Jinyi,Feng Quanyou,Huang Wei
Fully π-conjugated polymers with rigid aromatic units are promising for flexible optoelectronic devices, but their inherent brittleness poses a challenge for achieving high-performance, intrinsically stretchable fully π-conjugated polymer. Here, we are establishing an external-plasticizing strategy using semiconductor fluid plasticizers (Z1 and Z2) to enhance the optoelectronic, morphological, and stretchable properties of fully π-conjugated polymer films for flexible light-emitting diodes. The synergistic effect of hierarchical structure and optoelectronic properties of Z1 in poly(9,9-di-n-octylfluorene-alt-benzothiadiazole) (F8BT) films enable excellent stretchable deformability (~25%) and good conductivity. PLEDs based on F8BT/Z1 films show stable electroluminescence and efficiency under 15% stretch and 100 cycles at 10% strain, revealing outstanding stress tolerance. This strategy is also improving the stretchable properties of polymers like poly(9,9-di-n-octylfluorenyl-2,7-diyl) (PFO) and poly(2-methoxy-5(2′-ethyl)hexoxy-phenylenevinylene) (Super Yellow), demonstrating its general applicability. Therefore, this strategy can provide effective guidance for designing high-performance stretchable fully π-conjugated polymers films for flexible electronic devices.
研究领域:
材料科学
·
光学工程
✓ 已验证
DOI
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 11
·5072-5079
·
IF 6.97
Ting Geng,Tanglue Feng,Zhiwei Ma,Ye Cao,Yaping Chen,Songyuan Tao,Guanjun Xiao,Siyu Lu,Bai Yang,Bo Zou
The photoluminescence (PL) mechanism plays a significant role in the study of carbonized polymer dots (CPDs). The supramolecular interaction exists in most materials, which offers innate methods to regulate the optical and physical properties. However, insights into the tunable red- and blue-shifted PL peaks of CPDs by the supramolecular interaction still remain elusive. Herein, the supramolecular interaction-triggered fluorescence change of CPDs is reported by the investigation of the piezochromic behaviors. The π-conjugated system and the hydroxy group are both critical to manipulate the PL of CPDs under high pressure. The π–π stacking of the π-conjugated system was enhanced with increasing pressure, which induces the red-shifting of PL peaks, while the hydroxyl-related hydrogen bond formation eventually causes a blue-shift. In addition, their chemical stability, low toxicity, and the tunable PL properties of CPDs by supramolecular interaction under high pressure would deepen the understanding of the fluorescence mechanism of CPDs, inspiring extensive application prospects in sensing and light-emitting diodes.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Xinyuan Zhang,Xiaoguang Du,Jinhui Wang,Fangyan Wang,Fei Liang,Zhanggui Hu,Zheshuai Lin,Yicheng Wu
The delocalized π-conjugated units are considered as an advantageous gene for improving the optical nonlinearity of acentric crystals. For the first time, we synthesized a new acentric SHG-active metal cyamelurate crystal K3C6N7O3·2H2O (I) by a facile solution method, containing a colossal planar π-conjugated (C6N7O3)3– unit. It displays a strong second-order harmonic generation (SHG) of 4 × KDP and a giant anisotropic birefringence of 0.446 at 1064 nm. The theoretical calculations reveal that such substantial improvement is contributed from the strong molecular susceptibility of (C6N7O3)3– units and their near-perfect coplanar arrangement. Moreover, I exhibits a broadband ultraviolet photoluminescence at 366 nm, suggesting its multifunctional capacity and great potential for compact highly integrated optoelectronic devices.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 35
·15281-15286
·
IF 2.7
Tao Ouyang,Xu Chen,Shanshan Chen,Yanqiang Li,Xiaoying Shang,Zhiyong Bai,Ningtao Jiang,Zhishuo Yan,Junhua Luo,Sangen Zhao
Finding a deep-ultraviolet (deep-UV, λ < 200 nm) nonlinear optical (NLO) crystal is vital to a number of advanced optical technologies, yet it remains a great challenge. Herein, we report a deep-UV NLO crystal, K2B3O3F4(OH) (KBOFH), composed of π-conjugated confined groups. It exhibits a relatively large birefringence of 0.054@550 nm and a wide transparency window with an absorption edge below 200 nm. Theoretical calculations reveal that the observed optical properties of KBOFH originate from the confined π-conjugated [B3O3F4(OH)] unit, in which the π-conjugated interactions are decoupled by the tetrahedral non-π-conjugated [BO2F2] unit. This work provides an opportunity to design deep-UV NLO crystals containing π-conjugated confined groups.
研究领域:
材料科学
·
光学
·
固体物理
·
晶体工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）