Advanced Optical Materials
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2020
·Vol. 8
·期 21
·2001072
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IF 8.286
Ping Liu,Yuan Liu,Siwei Zhang,Jingzhou Li,Chunyun Wang,Cong Zhao,Pengbo Nie,Yuhan Dong,Xuan Zhang,Shixi Zhao,Guodan Wei
Lead-free single crystal perovskite materials exhibit impressive characteristics, such as high carrier mobility, low trap density, and long diffusion length. Herein, the high-performance blue light photodetectors are reported based on lead-free all-inorganic Cs 3 Sb 2 Br 9 perovskite single crystals. These millimeter-sized Cs 3 Sb 2 Br 9 single crystals have small thermal activation energy of 56.8 meV estimated by temperature-dependent photoluminescence study. There is no obvious structural phase transition of the as-obtained Cs 3 Sb 2 Br 9 single crystals since no Raman peak shift is observed with temperature increasing from 80 to 300 K. The as-constructed high quality Cs 3 Sb 2 Br 9 single crystals photodetectors have an excellent performance of a responsivity of 2.29 A W −1 , a sharp detectivity of 3.77 × 10 12 Jones, and an external quantum efficiency (EQE) peak of 1.8 × 10 3 %. Moreover, the photodetectors exhibit a fast response time (<0.2 ms) and the full width at half maximum (FWHM) of the sharp EQE peak is as narrow as 15 nm. This work provides a promising strategy in the design of lead-free, stable, and high-performance perovskites for photodetector devices.
研究领域:
材料科学
·
光学工程
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Kunlun Jiang,Wenjian Yang,Zhaobing Zhang,Yongli Zhang,Jing Lan,Dehao Chen,Wenzhe Li,Jiandong Fan
Cs3Sb2Br9, as a sort of novel lead-free perovskite single crystal, has the merits of high carrier mobility and a long diffusion length. However, the large-sized and high-crystallized Cs3Sb2Br9 single crystals are not easily obtained. Herein, we apply the vertical Bridgman method to grow centimeter-sized Cs3Sb2Br9 single crystal. The temperature-dependent crystal structure of Cs3Sb2Br9 is in situ characterized in the temperature range of 100–400 K. A novel crystallographic and electronic structure anisotropy of the as-grown Cs3Sb2Br9 single crystal along the transmission directions of [100] and [001] is experimentally and theoretically proved. Owing to the layered two-dimensional (2D) structure of Cs3Sb2Br9, quantum confinement effects prolong the lifetime of hot carriers, leading to their accumulation within the Sb–Br plane along the [100] direction, thereby resulting in a higher density of electronic states. Accordingly, the [100] device exhibits a carrier mobility higher than that of the [001] device, with the [100] device mobility being 4 orders of magnitude higher than that of the [001] device at 423 K, showing a remarkable anisotropy. The [100] device also shows responsivity ∼10 times higher than that of the [001] device.
研究领域:
材料科学
·
物理化学
·
半导体器件
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DOI
PubMed
高影响因子
Solar RRL
·
2021
·Vol. 5
·期 12
·2100559
·
IF 8.582
Hong-Hong Zhang,Zi-Chun Zhou,Yu-Jie Dong,Li Zhang,Hong-Yan Chen,Dai-Bin Kuang
Utilizing halide perovskites for photocatalytic aromatic C( sp 3 ) H bond activation remains a great challenge due to the serious recombination of photogenerated charge carriers and slow reaction dynamics of the materials themselves. Herein, a lead-free perovskite-based hybrid of Cs 3 Sb 2 Br 9 /g-C 3 N 4 nanosheet is constructed and applied for photocatalytic aromatic C( sp 3 ) H bond activation, which shows enhanced photocatalytic performance. By introducing ultrathin g-C 3 N 4 nanosheets as the heterogeneous nucleation sites, size-reduced and well-dispersed Cs 3 Sb 2 Br 9 nanocrystals can be obtained. The as-formed close contact and high-quality heterointerface between Cs 3 Sb 2 Br 9 and g-C 3 N 4 provides pathways for fast charge transfer which is beneficial to improve the separation efficiency of photogenerated electron−hole pairs. Under visible light irradiation, the Cs 3 Sb 2 Br 9 /g-C 3 N 4 hybrid photocatalyst can effectively oxidize toluene toward benzaldehyde and benzyl alcohol with a total conversion rate of 8346.8 μmol g −1 h −1 , which is 26.6- and 6.0-fold that of pure g-C 3 N 4 and Cs 3 Sb 2 Br 9 , respectively. This work demonstrates the potential of all-inorganic lead-free halide perovskite-based heterostructures for photocatalytic organic reactions.
研究领域:
材料科学
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化学
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光催化
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纳米技术
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Tao Shan,Sunzai Ke,Xin Yang,Xuhui Yang,Bo Weng,Lijuan Shen,Min-Quan Yang
Photocatalytic selective oxidation of aromatic hydrocarbons plays an important role in the production of value-added chemicals. A key step in this process is the activation of C(sp 3 )-H bond by photogenerated holes. However, the inadequate hole generation and lack of surface adsorption-activation sites severely hinders the improvement in photocatalytic C-H bond oxidation. In particular, the random charge migration to the surface impedes the effective capture of holes by surface active sites to dissociate the C(sp 3 )-H bond. Here, we design and fabricate a Co 3 O 4 /Cs 3 Sb 2 Br 9 p-n heterojunction that effectively addresses these challenges. The p-n heterojunction forms strong built-in electric fields (BEF) facilitating spatial charge separation. Holes are accumulated on Co 3 O 4 , while electrons are accumulated on Cs 3 Sb 2 Br 9 , thereby offering abundant active holes and electrons. Moreover, Co 3 O 4 shows stronger adsorption and activation capacity for the C(sp³)-H bond, enabling the C(sp 3 )-H bond dissociation with low reaction energy barrier. Consequently, the holes are directionally extracted from photoactive Cs 3 Sb 2 Br 9 to catalytically active Co 3 O 4 under visible light irradiation, thereby accelerating the toluene oxidation. The optimized 5 % Co 3 O 4 /Cs 3 Sb 2 Br 9 exhibits a benzyl aldehyde (BAD) evolution rate of 5044 μmol g −1 h −1 and a benzyl alcohol (BA) production rate of 1820 μmol g −1 h −1 , which are 12 and 17 times higher than that of blank Cs 3 Sb 2 Br 9 , respectively.
研究领域:
材料科学
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化学工程
·
光化学
·
催化
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Qi Qin,Cheng-Yi Huang,Zhi-Hua Xia,Wei-Qi Liu,Hong-Yan Chen,Dai-Bin Kuang
Rational modulation of interfacial electronic structure has been regarded as an appealing strategy to achieve effective charge separation and synergistic active-site cooperation in heterojunction photocatalysts, yet it remains a significant challenging. In this study, two-dimensional (2D) vinylene-linked conjugated covalent organic polymer (COP) functionalized with –F and –CN groups was designed through Knoevenagel condensation reaction. The influence of these groups on the interfacial properties and the photocatalytic performances of Cs 3 Sb 2 Br 9 /COP heterojunction were investigated systematically. Combined experimental and theoretical calculations revealed that introducing strong electron-withdrawing groups improves charge separation by inducing strong electron delocalization within the COP framework, enhances CO 2 adsorption and activation, and most importantly, significantly facilitates the interfacial growth of Cs 3 Sb 2 Br 9 nanocrystals. It was found that the strengthened interfacial interaction via Sb─N bonding effectively promoted a fast Z-scheme charge transfer and enabled effective spacial separation of photoelectron and holes, in contrast to the type II mechanism observed in the un-functionalized heterojunction. This enables effective multifunctional collaboration of Cs 3 Sb 2 Br 9 and FN-COP. Consequently, the optimized Cs 3 Sb 2 Br 9 /FN-COP heterojunction achieved a total electron rate of 135.42 µmol·g -1 ·h -1 for CO 2 reduction coupled with a benzaldehyde production rate of 179.73 µmol·g -1 ·h -1 , representing a 2.4 and 2.6-fold enhancement over the un-functionalized heterojunction. This work demonstrates a novel "molecular engineering–interface modulation–function cooperation" strategy to construct high-quality heterojunction precisely, providing valuable insights for the design of high-performance photocatalysts for next-generation energy conversion applications.
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高影响因子
CERAMICS INTERNATIONAL
·
2026
·
IF 6
Yalin Yang,Wei Lu,Yunsheng Xu
The selective oxidation of styrene to styrene oxide (SO) is a pivotal transformation in fine chemical synthesis. Conventional thermocatalytic routes suffer from unresolved critical issues: overoxidation, poor selectivity, and environmental incompatibility. Herein, a Cs 3 Sb 2 Br 9 (CSB)/TiO 2 composite photocatalyst was constructed by coupling lead-free halide perovskite CSB with wide-bandgap semiconductor TiO 2 for highly selective styrene epoxidation under mild conditions. CSB incorporation extends the composite's photoresponse to the visible region. Mechanistic investigations confirm that under visible-light excitation (λ > 420 nm), only CSB is photoexcited. Photogenerated electrons directionally transfer from CSB to the unexcited TiO 2 (acting as an electron mediator), These electrons reduce O 2 to ·O 2 - , while holes in CSB oxidize styrene and can convert ·O 2 - to 1 O 2 , shifting the reaction from C=C cleavage to selective epoxidation. At an optimal CSB loading of 0.18 mmol, the composite achieves a total reaction rate of 27.23 mmol ·g -1 ·h -1 (9.13-fold higher than pure TiO 2 ) and an SO selectivity elevated from 42.25% to 82.28%. Concurrently, the epoxide production rate reaches 22.40 mmol ·g -1 ·h -1 , representing 17.78-fold over that of pure TiO 2 (1.26 mmol·g -1 ·h -1 ). XPS analysis reveals a positive shift in Br 3d and negative shift in Ti 2p binding energies, verifying directional electron transfer from CSB to TiO 2 . Radical quenching experiments and EPR spectroscopy demonstrate that photogenerated electrons reduce O 2 to ·O 2 -, holes further convert ·O 2 - to 1 O 2 . This regulation of reactive oxygen species shifts the reaction pathway from competitive C=C bond cleavage to selective oxygen-transfer epoxidation. This work provides a novel material design strategy and mechanistic insights for constructing efficient, highly selective photocatalytic oxidation systems.
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高影响因子
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