Green Energy & Environment
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2021
·
IF 8.207
Dashui Yuan,Zongyuan Li,Xueru Chen,Jing Ding,Hui Wan,Guofeng Guan
Proper interface and band alignment always play essential roles in the separation of photoexcited charge of photocatalysts. In this work, we prepared a homodispersed S-scheme carbon nitride homojunction with local electron structure difference by a facile pre-doping and two-step calcination approach. Boron doping into heptazine created extra acceptor impurity, and phosphorus doping into heptazine created extra donor impurity, which eventually modulated the electronic structure of carbon nitride. As heptazines with different element doping were integrated into carbon nitride by recalcination, B–CN and P–CN formed a homodispersed homojunction and thus produced a rich interface. Meanwhile, caused by Fermi energy levels equilibrium, the band bending constructed an S-scheme homojunction, which stimulated photogenerated electrons to transfer from CB of B–CN to VB of P–CN. The homodispersed S-scheme homojunction structure led to efficient suppression of recombination of photoinduced charge and retained stronger redox charge. Consequently, the photocatalytic performance was dramatically boosted to 2620 μmol g −1 from 60 μmol g −1 of pure CN in 4-h hydrogen evolution from water. This novel method for electron structure engineering helped to provide a new strategy for designing homojunction photocatalysts with excellent photocatalytic performance.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-8
·
IF 12.121
Wang Chenhui,Han Dengbao,Wang Junhui,Yang Yingguo,Liu Xinyue,Huang Sheng,Zhang Xin,Chang Shuai,Wu Kaifeng,Zhong Haizheng
In the field of perovskite light-emitting diodes (PeLEDs), the performance of blue emissive electroluminescence devices lags behind the other counterparts due to the lack of fabrication methodology. Herein, we demonstrate the in situ fabrication of CsPbClBr 2 nanocrystal films by using mixed ligands of 2-phenylethanamine bromide (PEABr) and 3,3-diphenylpropylamine bromide (DPPABr). PEABr dominates the formation of quasi-two-dimensional perovskites with small- n domains, while DPPABr induces the formation of large- n domains. Strong blue emission at 470 nm with a photoluminescence quantum yield up to 60% was obtained by mixing the two ligands due to the formation of a narrower quantum-well width distribution. Based on such films, efficient blue PeLEDs with a maximum external quantum efficiency of 8.8% were achieved at 473 nm. Furthermore, we illustrate that the use of dual-ligand with respective tendency of forming small- n and large- n domains is a versatile strategy to achieve narrow quantum-well width distribution for photoluminescence enhancement.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Mina Yang,Haijing Zhang,Fei Chang,Xuefeng Hu
Chlorinated organic compounds are ubiquitously detected in saline waters. The photochlorination of organic compounds is one possible source, and chlorine radicals originating from other photosensitive substances have been reported to be responsible for organic compounds chlorination in previous reports. In this study, benzo[ a ]pyrene (BaP) chlorination in 10% acetonitrile/NaCl aqueous solution was initiated by self-sensitization of BaP, while chlorine radicals were not involved in the reaction. After 45 min of photoreaction in four seawater samples, chlorinated product (6-ClBaP) accounted for 10–17% of the fraction of transformed BaP, which was higher than that previously reported. The influences of Cl − , pH, humic acid , electron donors, and particulate matter on the formation of chlorobenzo[ a ]pyrene were systematically investigated. A self-sensitized photochlorination reaction mechanism was proposed as follow: photoexited BaP was activated to singlet state and then transformed to triplet state through inter-system crossing. Then the excited triplet state and oxygen formed [ 3 BaP*- 3 O 2 ] or [BaP- 1 O 2 ] complex, which further reacted with Cl − to produce 6-ClBaP.
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Advanced Optical Materials
·
2020
·Vol. 9
·期 1
·2001505
·
IF 8.286
Liang Chen,Sui Mao,Pu Wang,Zhao Yao,Zhonglin Du,Zhijun Zhu,Laurence A. Belfiore,Jianguo Tang
Hot-electron injection induced by plasmon decay enables ultrafast electron transfer in femtosecond scale and therefore endows metallic nanoparticles (MNPs) promising potentials in high-speed optoelectronics. With much higher density of states next to its Fermi level, palladium (Pd) can more efficiently launch hot electrons according to the theoretical prediction, as compared to the conventional plasmonic NPs. In this work, the optical properties of Pd NPs as well as the plasmon induced hot-electron injection are investigated through confocal Kelvin probe force microscopy. Analysis based on surface potential redistribution suggests Pd NPs can initiate dense hot-electron transfer in visible range. According to the photocurrent characterization of photo field effect transistors, in cooperation with TiO x the Pd NPs launch a rapid photocurrent increase with the excitation of 450 nm light as the hot-electron injection improves the electron depleting situation in TiO x thin film. The result confirms that Pd hot electrons can be energetic at visible range for photoelectric applications.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Fei Yang,Tongming Chen,Xiaoju Wu,Yuan Chen,Guowei Yang
Carbyne nanocrystals (CNCs), carbon materials with one-dimensional sp-hybridized atoms, have been synthesized in our lab, and these novel carbon nanomaterials exhibit unique physical and chemical properties. Here, we report that CNCs capped with gold nanoparticles (CNCs@AuNPs), a hybrid nanostructure platform, possess dual-enzyme mimetic properties of peroxidase (POD) and superoxide dismutases (SOD), catalyzing the reduction of hydrogen peroxide (H 2 O 2 ) to initiate a characteristic color reaction at acidic pH and the disproportionation of O 2 − producing O 2 and H 2 O 2 at alkaline pH, respectively. Interestingly, upon exposure to light, AuNPs catalyze the oxidation of oxidase (OD) substrates with the involvement of CNCs. The mechanism of the catalytic process was analyzed by measurements of the produced species and electrons. These findings make CNCs@AuNPs promising enzyme mimetic candidates and expand their applications in redox catalysis, bioassays and photodynamic therapy.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yangjie Fu,Kejie Zhang,Yi Zhang,Yanqing Cong,Qi Wang
Visible-light-active MR/NH 2 -MIL-125(Ti) homojunction was successfully synthesized via post-synthetic modification of NH 2 -MIL-125(Ti). A chromophore group (–MR) similar to the structure of methyl red, was introduced to partially replace the –NH 2 group. Using pure NH 2 -MIL-125(Ti) and MR-MIL-125(Ti) as control samples, the possible structural and optical changes were carefully studied. It was found that the lattice structure remained unchanged, while the specific surface area and band gap were in the order of NH 2 -MIL-125(Ti) > MR/NH 2 -MIL-125(Ti) > MR-MIL-125(Ti). Despite of these, MR/NH 2 -MIL-125(Ti) exhibited highest photocurrent response and lowest charge transfer resistance, which were associated with optimal photocatalytic performance. For the photocatalytic reduction of Cr(VI), the estimated rate constant on MR/NH 2 -MIL-125(Ti) was ca. 9 times and 3 times relative to that on NH 2 -MIL-125(Ti) and MR-MIL-125(Ti), respectively. Besides, 4.6 times rate enhancement can also be observed on the homojunction relative to physical mixture (MR/NH 2 -MIL-125(Ti)-PM). The boosted photocatalytic performance may be ascribed to promoted separation and transfer of photogenerated electron-hole pairs. The operating factors was optimized at acidic pH (2.0), lower catalyst dosage (0.1 g/L) and appropriate concentration of coexisting organics (2.0 mM) within the tested range. Furthermore, good stability both in photocatalytic performance and structure were also observed after 5 cyclic runs. Thus, this study report a facile way for the construction of visible-light-active MOFs, and provided a stable photocatalytic candidate for the disposal of Cr(VI)-containing wastewaters.
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Materials Research Express
·
2021
·Vol. 8
·期 2
·025902
·
IF 1.62
Dong Zhang,Bingjun Zhu,Shiqi Ren,Qingru Wang,Qinglin Wang,Shuhong Li,Bingyuan Zhang,Wenjun Wang
ZnAl2O4 with spinel structure has attracted more attentions due to its robust dielectric and luminescence properties. Complex cation distribution in spinel structure influences the optical and magnetic properties. Herein, we report white emission related to the defects and the magnetism assigned to Fe impurity in ZnAl2-xFexO4 (0\leqslant x\leqslant 0.6) nanocrystals fabricated by using common sol-gel method at a relatively lower temperature (700 °C) than that reported earlier. ZnAl2-xFexO4 phosphors reveal single spinel phase without impure phase. Complex cation distribution is observed in all samples, for instance, Fe and Zn in antisites, cation vacancies, and with Fe content increasing, cation distribution reveals obvious change. The band gap energy of ZnAl2-xFexO4 phosphors is reduced from 3.84 eV to 3.33 eV when the content of Fe ions (x value) increases from 0 to 0.6. Two wide band emissions assigned to the various types of shallow and deep donor/acceptor defects are observed, monitoring with the excitation wavelength of 280 nm. The Commission International de I'Eclairage (CIE) colour coordinate (x, y) of the ZnAl2-xFexO4 phosphors is found to shift from (0.3218, 0.2957) to (0.3422, 0.3122) with Fe doping in spinel lattices owing to rearrangement of defects, indicating the potential application in white-light illumination. ZnAl2-xFexO4 reveals a room ferromagnetism resulting from Fe3 + ions in spinel lattices.
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COMPOSITES SCIENCE AND TECHNOLOGY
·
2021
·
IF 8.528
Yan-Qin Wang,Yu Zhu,Jing-Hui Wang,Xiao-Na Li,Xiao-Gang Wu,Yi-Xian Qin,Wei-Yi Chen
Recently, artificial intelligence has driven the development of shape memory hydrogels (SMHs) with complicated environmental sensitive abilities. However, current SMHs possess fundamental limitations in terms of their responsive performance and mechanical properties , which severely limits their practical applications. Herein, a triple-network composite hydrogel with Fe 3+ , NIR light, and thermal responsive abilities is fabricated and developed as multi-SMHs, named as PDA/CMC-Fe 3+ /PVA hydrogel. In this hydrogel system, the interpenetrating triple network are formed by chemically-physically co-crosslinked polyvinyl alcohol (PVA) networks, and physically crosslinked carboxymethyl cellulose (CMC)-Fe 3+ network. In addition, polydopamine (PDA), which is introduced into the hydrogel system by in-situ polymerization way, could not only serve as an energy converter to endow the hydrogel with NIR-based responsive ability, but also enhance its mechanical strength . Remarkably, the as-prepared PDA/CMC-Fe 3+ /PVA hydrogels with the optimized compositions exhibit relatively excellent mechanical properties (tensile strength = 163.48 ± 10.42 kPa, elastic modulus = 45.42 ± 3.96 kPa, toughness = 165.02 ± 7.01 kJ/m 3 ) due to the synergistic effect of the triple-network and PDA doping. Moreover, the composition of the hydrogel is optimized to realize a stable temporary shape and rapid recovery to the permanent shape, which is controlled by Fe 3+ , NIR irradiation, and thermal stimulus. The resultant hydrogels exhibit not only multi-stimulus responsive abilities, but also programmable multi-shape memory properties. The versatile shape memory properties endow potential for the materials to be used in the field of artificial intelligence.
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BIOMATERIALS
·
2020
·
IF 10.317
Guannan Zhang,Yongqiang Yang,Jing Shi,Xiaohong Yao,Weiyi Chen,Xiaochun Wei,Xiangyu Zhang,Paul K. Chu
Light-triggered therapy is a prospective method to combat implant-associated infection but near-infrared I (NIR-I) light has insufficient penetrating ability in tissues and local hyperthermia induced by the photothermal treatment may destroy surrounding healthy tissues. Herein, a near-infrared II (NIR-II) phototherapy system composed of upconversion elements doped titanium dioxide nanorods (TiO 2 NRs)/curcumin (Cur)/hyaluronic acid (HA)/bone morphogenetic protein-2 (BMP-2) is designed for biomedical titanium and demonstrated to overcome the above hurdles simultaneously. Incorporation of F, Yb, and Ho not only improves the photocatalytic ability, but also renders the implants with the upconversion capability, so that the NRs can generate enough reactive oxygen species (ROS) when irradiated by the NIR-II laser . Furthermore, the combined actions of quorum sensing inhibitors, ROS, and physical puncture by NRs eliminate Staphylococcus aureus biofilms on titanium rapidly at a mild temperature of 45 °C by only requiring irradiation with the 1060 nm laser for only 15 min in vitro and in vivo . The presence of Cur mitigates the immune response and BMP-2 improves osteogenic differentiation , thus accelerating new bone formation. This low-temperature NIR-II light-triggered antibacterial platform has large potential in combating deep-tissue infection in clinical applications.
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Journal of Physical Chemistry C
·
2020
·
IF 4.189
Siqi Sun,Min Lu,Jie Guo,William W. Yu,Zhifeng Shi,Guang Sun,Yu Zhang
Improved device performance of perovskite light-emitting diodes (LEDs) is demonstrated through the synergistic effect of the optimized CsPbI3 nanocrystals (NCs) as the emissive layer (EML) and ZnO/C60 bilayer as electron transport layers (ETLs). The optical characteristics of the CsPbI3 NCs were optimized by strictly controlling the feeding ratio of Cs:Pb:I to 1:1:3 in the synthesis processes of NCs, which leads to enhanced photoluminescence quantum yields (PL QY) from 65% to 92%. Additionally, the introduction of C60 not only optimized the energy level structure of the device, leading to more balanced charge injection and transport, but also smoothed the surface of the ZnO film and perovskite NCs. Consequently, a peak external quantum efficiency (EQE) of 10.7% and maximum luminance of 1377 cd m–2 were achieved.
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Journal of Materials Chemistry C
·
2020
·Vol. 9
·期 3
·916-924
·
IF 7.059
Guangrong Jin,Dengliang Zhang,Peiyuan Pang,Ziqing Ye,Tanghao Liu,Guichuang Xing,Jiangshan Chen,Dongge Ma
Quasi-2D CsPbBr3 perovskites hold great potential as the promising emitters for perovskite light-emitting diodes (PeLEDs) owing to their good film morphology, excellent thermal stability and efficient radiative recombination. However, quasi-2D CsPbBr3 films are usually composed of multiple phases with various numbers (n) of [PbBr6]4− octahedral layers, and the formed n = 1 phase shows nonradiative recombination and retarded exciton transfer, which are detrimental to the performance of PeLEDs. Here, we report a facile approach to grow quasi-2D CsPbBr3/Cs4PbBr6 nanocomposite films as the emissive layers (EMLs) for efficient PeLEDs by simply introducing excess CsBr in the precursor solution. In the perovskite nanocomposite films, it is found that the formation of the n = 1 phase is completely suppressed and the density of trap states is dramatically lowered, leading to the significant reduction of nonradiative losses. In addition, the formed Cs4PbBr6 with a large bandgap can centralize carriers and confine excitons in quantum wells to realize efficient transfer, and can also constrain the crystal size and enhance the exciton binding energy of CsPbBr3, all of which facilitate the radiative recombination. As a result of the reduced nonradiative losses and improved radiative recombination, the green PeLED based on the quasi-2D CsPbBr3/Cs4PbBr6 nanocomposite EML achieves greatly enhanced performance with a maximum external quantum efficiency (EQE) of 11.84%, which is much higher than the maximum EQE of 1.94% of the quasi-2D CsPbBr3 device. This study demonstrates that the construction of perovskite nanocomposites should provide an effective way to promote the performance of PeLEDs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Wenya Xu,Wen Wang,Simou Chen,Rui Zhang,Yuxin Wang,Qi Zhang,Lihui Yuwen,Wen Jing Yang,Lianhui Wang
The fabrication of flexible electronic sensors with self-healing capability is of great importance for the applications in wearable devices and skin-like electronics. Herein, a molybdenum disulfide (MoS 2 ) nanosheets-based hydrogel (Gel-PEG-MoS 2 , GPM hydrogel), with near infrared (NIR) light-induced self-healing property, was first reported as a flexible sensor. Only a small amount of MoS 2 nanosheets (0.04 wt‰) could impart the hydrogel with fast self-healing property under NIR irradiation in 90 s. The healing efficiencies increased with the increasing of MoS 2 loadings. Moreover, the GPM hydrogel exhibited both contact and noncontact sensing properties based on its deformation-dependent and light-sensitive conductivity, showing potential application as mechanical sensor and light-activated switches. By employing the versatile MoS 2 nanosheets, the hydrogel exhibited both fast self-healing ability and mechanical/light sensing capability. Therefore, the MoS 2 -based hydrogel provides a two-pronged approach for construction of self-healing flexible electronics.
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