Materials Today Communications
·
2023
·
IF 3.8
Yun Tang,Yuchao Zhang,Ben Liu,Xiaoqiang He,Hudie Yuan,Yalou Xin
Polymer encapsulation is regarded as an efficient strategy to enhance the stability of perovskite quantum dots (PQDs), and also endows the perovskites with advantages in mechanical properties and processibility. In this work, polymer encapsulation was achieved by in-situ synthesis of PQDs in polycaprolactone (PCL) polymer, which avoiding time-consuming process of blending polymer with PQDs. Moreover, besides of acting as encapsulation matrix, PCL in toluene could provide large nucleation sites for PQDs formation, resulting in the relatively smaller PQDs size and enhanced photoluminescence quantum yield (PLQY) with respect to the composites prepared by physical blending. Profiting from PCL encapsulation, the as-synthesized PQDs-PCL composites exhibited enhanced stability against UV light, water and heat. The strong interaction between PQDs and PCL in composites with high PCL concentration could endow them with more significantly improved PL stability under UV-light illumination and relatively better mechanical properties compared to the composites with high PQDs concentration. This work provides an efficient method to synthesize PQDs-polymer composites with enhanced PLQY and stability, which would promote practical applications of PQDs materials in the optoelectronic applications .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yuan Teng,Jing-Hua Chen,Yu-Hua Huang,Zi-Chun Zhou,Xu-Dong Wang,Dai-Bin Kuang,Hong-Yan Chen
The construction of high-quality heterojunction with staggered band structure and close-contact interface, to satisfy both the thermodynamic and dynamic prerequisites of charge transfer, is the key to improve the charge separation of halide perovskites . The in situ growth of perovskite heterojunction via cosharing atoms provides an appealing solution to tackle this dilemma, but it remains a big challenge owing to the lack of appropriate precursors. Here, we design a novel visible-light responsive Co x Bi 2−x O 2 CO 3 nanosheet , and use it as self-template to epitaxially grow Cs 3 Bi 2 Br 9 nanosheet . It is revealed that close-contact 2D/2D heterointerfaces with strong chemical and electronic coupling are built via Bi atom bridge. Moreover, incorporating Co 3+ into Bi 2 O 2 CO 3 plays critical roles in heterojunction growth by regulating both the electronic structure and growth dynamics of Cs 3 Bi 2 Br 9 . Triggered by the effect of Co and the matched Bi lattice with Cs 3 Bi 2 Br 9 , the Co x Bi 2−x O 2 CO 3 /Cs 3 Bi 2 Br 9 heterojunction can drive the fast Z-scheme transfer and separation of photoexcited charge carriers.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Yang Tinghuan,Gao Lili,Lu Jing,Ma Chuang,Du Yachao,Wang Peijun,Ding Zicheng,Wang Shiqiang,Xu Peng,Liu Dongle,Li Haojin,Chang Xiaoming,Fang Junjie,Tian Wenming,Yang Yingguo,Liu Shengzhong (Frank),Zhao Kui
Even though the perovskite solar cell has been so popular for its skyrocketing power conversion efficiency, its further development is still roadblocked by its overall performance, in particular long-term stability, large-area fabrication and stable module efficiency. In essence, the soft component and ionic–electronic nature of metal halide perovskites usually chaperonage large number of anion vacancy defects that act as recombination centers to decrease both the photovoltaic efficiency and operational stability. Herein, we report a one-stone-for-two-birds strategy in which both anion-fixation and associated undercoordinated-Pb passivation are in situ achieved during crystallization by using a single amidino-based ligand, namely 3-amidinopyridine, for metal-halide perovskite to overcome above challenges. The resultant devices attain a power conversion efficiency as high as 25.3% (certified at 24.8%) with substantially improved stability. Moreover, the device without encapsulation retained 92% of its initial efficiency after 5000 h exposure in ambient and the device with encapsulation retained 95% of its initial efficiency after >500 h working at the maximum power point under continuous light irradiation in ambient. It is expected this one-stone-for-two-birds strategy will benefit large-area fabrication that desires for simplicity.
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Materials Today Chemistry
·
2022
·
IF 7.613
Yipin Zhang,Chenyang Qi,Jing Tu
The poor stability and low reusability of enzymes have always been the hindrances to their large-scale applications. Herein, hollow mesoporous silica (HMS) nanoparticles have been constructed as nanoreactors for in situ enzyme immobilization, hemoglobin (Hb) was selected as a model enzyme. By utilizing zeolitic imidazolate framework-8 (ZIF-8) as the sacrificial template, the synthesis mechanism of Hb@ZIF-8 has been explored by adjusting the molar ratios of Zn 2+ and 2-methylimidazole. When the amount of Hb was constant, the shape of Hb@ZIF-8 gradually changed from flake to granular (from 50:200 mM to 50:800 mM). Furthermore, when the molar ratio of Zn 2+ and 2-methylimidazole was fixed, with the amount of Hb increasing, the size of Hb@ZIF-8 decreased gradually, with maximum loading capacity of 460 μg/mg. Subsequently, Hb@ZIF-8 was coated with silica shells and followed by the removal of ZIF-8 in phosphate-buffered saline (pH 5), resulting in Hb@HMS. Compared to free Hb, Hb in HMS nanoreactors maintained over 74% of original catalytic activity under extreme conditions, showing significant improvements on the stability. Further, Hb@HMS still retains 80% of enzymatic activity after 5 cycles, exhibiting its excellent reusability. This work provides an efficient strategy for enzyme immobilization, giving new horizons for biosensing, biocatalysis and biomedicine.
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JOURNAL OF LUMINESCENCE
·
2022
·
IF 4.171
Yanqing Zhu,Cong Shen,Xueqing Xu,Jianhua Zou,Lei Wang,Xudong Cheng,Jingqiu Liang,Xiudi Xiao,Gang Xu
InP quantum dots (QDs) with low toxicity are considered to be the most promising materials. However, the oxidation problem of In and P has become to the major factor affecting the optical properties of InP QDs. In this work, the effect of luminescence properties of InP/GaP/ZnS QDs with halogen acid treatment have been studied. The results show that HF and HCl are beneficial to improve the optical properties of QDs, HBr especially HI are not conductive to promote the photoluminescence quantum yield (PL QY) of QDs. HF and HCl can etch the oxidative layer effectively, the F − and Cl − can also passivate the surface indium dangling bonds in the form of atomic ligands. The proposed model of charge carrier recombination show that the PL QY improved significantly after HA treatment attributed to the recombination of electron-hole pairs through radiative pathways mainly from the conduction band and valence band . The InP QDs with HF treatment has the best luminescence properties with high PL QY of 96%, offering great potential for advanced optoelectronic devices.
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Micromachines
·
2022
·Vol. 14
·期 1
·11
·
IF 3.523
Weigao Wang,Yiyang Li,Yu Duan,Mingxia Qiu,Hua An,Zhengchun Peng
Poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) is widely used in optoelectronic devices due to its excellent hole current conductivity and suitable work function. However, imbalanced carrier injection in the PEDOT:PSS layer impedes obtaining high-performance perovskite light-emitting diodes (PeLEDs). In this work, a novel poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,40-(N-(p-butylphenyl))diphenylamine)] (TFB) is applied as the hole transport layers (HTLs) to facilitate the hole injection with cascade-like energy alignment between PEDOT:PSS and methylammonium lead tribromide (MAPbBr3) film. Our results indicate that the introduced TFB layer did not affect the surface morphology or lead to any additional surface defects of the perovskite film. Consequently, the optimal PeLEDs with TFB HTLs show a maximum current efficiency and external quantum efficiency (EQE) of 21.26 cd A−1and 6.68%, respectively. Such EQE is 2.5 times higher than that of the control devices without TFB layers. This work provides a facile and robust route to optimize the device structure and improve the performance of PeLEDs.Keywords:lead halide perovskites;perovskite light-emitting diodes;hole transport layers;interface modification
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Yunlong Yang,Yuanlong Guo,Chengtao Gao,Michael North,Jili Yuan,Haibo Xie,Qiang Zheng
Cellulosic poly(ionic liquid)s ([Cellmim][Br]) with a degree of substitution (DS) in the range of 0.32–0.89 were synthesized successfully via the homogeneous transesterification reaction of cellulose with 1-(2-methoxyacetyl)-3-methyl imidazole bromide IL ([Mmim][Br]) in a DBU/DMSO/CO2 solvent system. The structure and properties of these novel materials have been fully characterized. Cellulosic poly(ionic liquid) POF polymers (POF-[Cellmim][Br]) were then obtained by an in situ crosslinking reaction without adding an exterior catalyst. The porosity and properties of the POF-[Cellmim][Br] materials can be modulated. The POF-[Cellmim][Br] materials functioned as green, efficient, and highly active catalysts for cycloaddition reactions of epoxides and carbon dioxide under solvent-free and co-catalyst-free conditions. These reactions gave high yields (up to 97%), and the catalyst can be easily separated with excellent reusability and no significant change to its structure. A plausible reaction mechanism for the cycloaddition reaction of epoxide and carbon dioxide by the POF-[Cellmim][Br] catalyst is proposed based on the experimental results. This work provided a new strategy to prepare cellulosic-PIL POF materials and offered a platform to understand the cooperative effects of porous properties and nucleophilic anions on the cycloaddition reaction of carbon dioxide and epoxides.
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Small
·
2023
·Vol. 19
·期 16
·2207393
·
IF 13.3
Lina Hua,Liwei Tang,Yi Liu,Shiguo Han,Haojie Xu,Wuqian Guo,Yu Ma,Xitao Liu,Junhua Luo,Zhihua Sun
The bulk anomalous photovoltaic (BAPV) effect of acentric materials refers to a distinct concept from traditional semiconductor-based devices, of which the above-bandgap photovoltage hints at a promise for solar-energy conversion. However, it is still a challenge to exploit new BAPV-active systems due to the lacking of knowledge on the structural origin of this concept. BAPV effects in single crystals of a 2D lead-free double perovskite, (BBA) 2 CsAgBiBr 7 ( 1, BBA = 4-bromobenzylammonium ), tailored by mixing aromatic and alkali cations in the confined architecture to form electric polarization are acquired here. Strikingly, BAPV effects manifested by above-bandgap photovoltage ( V OC ) show unique attributes of directional anisotropy and positive dependence on electrode spacing. The driving source stems from orientations of the polar aromatic spacer and Cs + ion drift, being different from the known built-in asymmetry photovoltaic heterojunctions. As the first demonstration of the BAPV effect in the double perovskites, the results will enrich the family of environmentally green BAPV-active candidates and further facilitate their new optoelectronic application.
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Advanced Electronic Materials
·
2023
·Vol. 9
·期 3
·2201222
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IF 6.2
Kewen Tao,Chenwei Xiong,Jiachun Lin,Decai Ma,Shaopeng Lin,Biao Wang,Huashan Li
Self-powered halide perovskite X-ray detectors have evoked busting interests because they present outstanding properties such as low power consumption, high sensitivity, and integrability without external power source. Nevertheless, existing self-powered X-ray detectors exhibit low sensitivity due to the insufficient charge separation and transport. Herein, a self-powered photodetector for sensitive X-ray and photodetection based on single-crystalline perovskite FAPbBr 3 /NiO x heterostructure is demonstrated. The built-in field of FAPbBr 3 /NiO x heterojunction provides a driving force for separation and transport of photoexcited carriers. Without an external power supply, the photodetector presents excellent photoresponse performance under 450 nm light illumination, including high photoresponsivity (123.6 mA W −1 ), good detectivity ( D = 7.1 × 10 11 Jones), and ultrafast response/recovery time (10/200 ns). Simultaneously, the device achieves photovoltaic effect of 0.80 V and a large mobility–lifetime product of 1.1 × 10 −3 cm 2 V −1 , which enable a superior X-ray sensitivity of 402 µC Gy air −1 cm −2 at zero bias voltage. These results imply that the simple combination of perovskite single crystal and a hole transporting layer provides a flexible platform for the realization of energy-saving self-powered photodetector in visible light and X-rays.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 14
·2213964
·
IF 19
Qin Chen,Haidong Jiang,Yipeng Fan,Zhou Li,Huang Ye,Yunpeng Yao,Shuang Chen,Chengmin Ji,Shuhua Zhang,Junhua Luo
Hybrid organic–inorganic perovskite (HOIP) ferroelectrics with high Curie temperature ( T c ), typified by the lead halide hybrid perovskite ferroelectrics, are developing rapidly owing to their maneuverable ferroelectricity at high temperatures. However, acquiring high- T c lead-free HOIP ferroelectrics via rational strategy still needs development. In this study, a brand-new program by modulating the steric confinement in a cuplike cavity to design high- T c bismuth-halide ferroelectrics [H 2 mdap]BiX 5 (H 2 mdap = N -Methyl-1,3-Propanediamine, X = Cl ( 1 ), Br ( 2 ), I( 3 )) is proposed. Emphatically, the T c enhanced dramatically from 264 K of 3 to 318 K of 2 and 377 K of 1 , induced by the substitution of Br and Cl to I, accompanied with an interesting transition from second-order phase transition (for 3 ) to the first-order one (for 1 and 2 ). The extent of T c increase is up to 113 K, which far outweighs that of reported Pb-halide hybrid ferroelectrics. Structural and computational analyses elucidate that this unprecedented improvement of T c is due to the higher phase transition energy barriers induced by modulating the steric confinement of cuplike cavity via halogen substitution. These results will provide new inspiration for designing high- T c lead-free HOIP ferroelectrics.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Nan He,Pifu Gong,Xingyu Zhang,Youquan Liu,Linfeng Dong,Zheshuai Lin
Hybrid organic–inorganic metal halide (OIMH) perovskites are regarded as potential photoluminescent (PL) materials and have attracted intensive attention. Here, we select 1-methylpiperazine as an organic component and successfully obtain a two-dimensional (2D) Ge-based OIMH perovskite, (1-mpz)GeBr4. It features a 2D layered structure composed of distorted [GeBr6]4– octahedra with organic (C5H14N2)2+ located between the layers. (1-mpz)GeBr4 exhibits strong orange color under ultraviolet (UV) light and possesses good PL stability for over 2 months. The photoluminescence quantum efficiency is measured to be 7.15% at room temperature, which is the largest among all reported low-dimensional Ge-based perovskites. Experimental measurements, combined with first-principles calculations, reveal that its PL property is attributed to self-trapped excitons (STEs) from [GeBr6]4– groups. From the deduced structure–property relationship, Ge-based OIMH PL perovskites with good stability and high PL efficiency can be expected.
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ACS Applied Electronic Materials
·
2023
·
IF 4.7
Yingjun Chai,Zhili Juan,Ye Wu,Yang Liu,Xiaoming Li
Metal halide perovskites have been demonstrated as potential X-ray detection materials due to their high defect tolerance, large diffusion length, and high attenuation efficiency. X-ray detectors based on hot-pressed perovskite wafers are investigated intensively recently because of the convenience of scalable fabrication. However, in spite of the large crystal size within wafers, the prepared detectors usually suffer from severe ion migration and current drift under both dark and bright states. In this work, ethylenediamine dihydroiodate (EDDI) was introduced as a strong surface passivation agent, which compensated for the surface iodide vacancy successfully. The ion migration in optimal MAPbI3@EDDI wafer is significantly suppressed, which is manifested by increased migration activation energy and stable current under high bias for 10 h. Moreover, the introduction of EDDI also reduced the dark current, contributing a high on–off ratio and a champion sensitivity of 8291.22 μC Gyair–1 cm–2. A low detection limit of 340 nGyair s–1 is also obtained, which is much lower than that of commercial X-ray detectors. Besides, the as-fabricated X-ray detector can endure long-term operation with flat current under a high bias of 20 V. This work provides a route for the performance improvement of perovskite wafer-based X-ray detectors.
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