JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2023
·Vol. 34
·期 9
·794
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IF 2.8
Li Ji,Xiang Peng,Tan Xinyu,Li Bowen,Zhang Kai,Zhu Ying,Ren Yanqi,Chen Xiaobo
Organic–inorganic lead halide peroxides (OIHPs) have attracted much interest due to their excellent photovoltaic properties, but practical applications are limited by long-term stability and further performance enhancement. Two-dimensional/three-dimensional (2D/3D) heterojunction is a promising strategy to address these issues. Here, short-chain 3,5-dichlorobenzylamine (DBA) with halogen functional groups is introduced to react with excess PbI 2 to form the 2D perovskite layer in mixed perovskite films of Cs 0.05 (FA 0.85 MA 0.15 ) 0.95 Pb(I 0.85 Br 0.15 ) 3 , which passivates surface defects, favours energy band alignment of functional layers and suppresses non-radiative recombination of carriers. As a result, DBA-treated 2D/3D PSCs obtained a champion PCE of 21.54% with an improved open circuit voltage ( V oc ) of 1.171 V. More importantly, the 2D/3D heterojunction can effectively protect the underlying 3D perovskite from moisture ingress. The unencapsulated 2D/3D devices retain 90% of their initial efficiency even after aging at 40 ± 5% RH for 1000 h, while the 3D device retains only 40%.
研究领域:
材料科学
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光伏技术
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纳米结构材料
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表面化学
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能源材料
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2026
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IF 8.7
Yuyan Xiao,Ningning Zhang,Aoqian Xi,Li Zhou,Yanning Zeng
Developing high-performance, closed-loop recyclable, and bio-based adhesives remains a significant challenge due to the inherent trade-off between crosslinking density and reprocessability. Herein, we report a bio-based vitrimer adhesive derived from peach gum polysaccharide (PGP) via vinylogous urethane (VU) chemistry. PGP was first modified with tert-butyl acetoacetate, followed by crosslinking with a fatty acid-derived diamine to form dynamic VU networks (PUV-x). The resulting PUV-1.0 network exhibits excellent mechanical properties (tensile strength up to 28.5 MPa, Young's modulus of 427.0 MPa, and elongation at break of 67.0%) and high thermal stability ( T s = 174.5 °C). Benefiting from the associative exchange of VU bonds, the material demonstrates rapid stress relaxation (activation energy of 30.4 KJ·mol −1 ), efficient self-healing (16 min at 100 °C) of surface scratches, and weldability. Moreover, the PUV-1.0 adhesive exhibits strong adhesion to various substrates (wood, steel, and glass), achieving an adhesion strength of up to 18.9 MPa on wood. It also maintains stable bonding performance under extreme temperatures (−22 to 100 °C) and in harsh environments (water, acid, alkali, sweater, and ethanol). The network can be chemically degraded and closed-loop recycled via transamination reactions, and the adhesive can be removed on demand from different substrates. This work provides a high-performance, and recyclable vitrimer adhesive platform, highlighting the potential of PGP in advanced bio-based materials.
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ACS Applied Nano Materials
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2023
·
IF 5.9
Wujiayue Luo,Junjie Chen,Yutong Sun,Zhenglin He,Yunzhang Li,Guosheng Shi
Ultrafast molecular-sieving graphene-based membranes with selective separation of volatile aromatic compounds (VACs) have great potential in environmental protection, reutilization of expensive materials, and industrial separation processes. However, current graphene-based absorbents suffer from slow removal speed and limited adsorption capacity for VACs. Herein, pristine and Ni2+-controlled graphene oxide membranes (GOMs) with a permeance up to ∼8.0 × 10–6 mol m–2 s–1 Pa–1, being 1–2 orders of magnitude higher than those of previously reported membranes. The GOMs selectively separate VACs from N2 is achieved on ceramic substrates via the size-exclusion effect for the first time. At a high VACs feed concentration, such GOMs show high rejection rates of 99.8, 99.4, 95.9, and 97.3% for phenol, benzaldehyde, benzoic acid, and benzylamine, respectively. X-ray diffraction (XRD) results show the two-dimensional (2D) channel size for gas transportation within the GOMs is 0.44 nm, which can reject the transportation of VACs but have no effect on N2. Interestingly, using improved Ni2+-controlled GOMs, the rejection rates of benzoic acid and benzylamine rejection rates increased from 95.9 to 98.6% and from 97.3 to 99.4%, respectively. Our finding provides a fast and efficient way to filter VACs in air and has potential applications in air purification and industrial processes.
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GREEN CHEMISTRY
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2023
·Vol. 25
·期 11
·4453-4462
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IF 9.8
Ye Meng,Jinshu Huang,Jie Li,Yumei Jian,Song Yang,Hu Li
Nitriles are versatile nitrogen-containing scaffolds that exist widely in medicines, dyes and functional materials, and are typically synthesized over homogeneous catalysts under relatively harsh conditions. Herein, through mimicking the key active species of hemoglobin p450 heme monooxygenase in most organisms, a Fe–N4 single atom-doped sulfur-containing carbon nitride (Fe/CNS) photocatalyst was facilely prepared by one-step thermal polymerization, which was illustrated to be efficient for renewable conversion of bio-based alcohols and NH2OH·HCl to a wide range of nitriles (80–92% yields) via cascade oxidation–ammoxidation at room temperature, or to quantitatively furnish benzaldehyde via oxidation in the absence of a nitrogen source. Theoretical calculations showed that the isolated Fe–N4 sites directly capture photogenerated electrons (e−) and molecular oxygen (O2) to generate superoxide radicals (˙O2−), while the surrounding S atoms confine photogenerated holes (h+). The high efficiency of Fe/CNS in the photo-generation of ˙O2− and holes may contribute to the smooth formation of nitriles by cascade photocatalytic oxidation of alcohol and ammoxidation via an in situ formed oxime, respectively. Moreover, Fe/CNS was also applicable to the selective synthesis of various imines (83–98% yields) from the oxidation of benzylamines or heterocyclic amines under visible-light irradiation, and could be recycled at least 5 times with no evident decline in catalytic activity. The strategy of rationally constructing atomic sites to spatially isolate paired electron–holes and form specific reactive species for enhanced photocatalytic activity/selectivity provides an efficient and green approach for biomass valorization.
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ANALYTICA CHIMICA ACTA
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2022
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IF 6.911
Ruiming Chen,Tingting Hu,Shu Xing,Tao Wei,Jianbin Chen,Tianduo Li,Qingfen Niu,Zhengyang Zhang,Huijun Ren,Xiaoxu Qin
Hydrazine (N 2 H 4 ) and hypochlorite (ClO − ) are extremely harmful to the public health, so it is vitally necessary to detect them in living system. Herein, we developed a new phenthiazine-thiobarbituric acid based dual-analyte responsive fluorescent sensor PT for visually distinguishing and detecting N 2 H 4 and ClO − . PT underwent N 2 H 4 /ClO − -induced C C breakage, achieving olive-drab/brilliant green fluorescence lighting-up response towards N 2 H 4 /ClO − with superb specifity, ultra-sensitivity (detection limit: 15.4 nM for N 2 H 4 , 13.7 nM for ClO − ), and ultra-fast response (N 2 H 4 : <15 s, ClO − : <20 s). The mechanisms for sensing N 2 H 4 and ClO − were investigated with support of spectral measurements and DFT investigation. Sensor based paper-strip/silica-gel device was developed for in-field supervision and on-site monitoring of gaseous and aqueous N 2 H 4 and ClO − solution. In addition, the PT was also applied for quantitatively detecting N 2 H 4 and ClO − in soil, food, plants and bio-fluids. Moreover, PT was utilized to visualize exogenous N 2 H 4 and ClO − in living plants and live-cells, demonstrating this sensor utilized as a powerful tool to detect N 2 H 4 and ClO − in biological fields.
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ACS Catalysis
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2023
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IF 12.9
Yaming Hao,Jili Li,Xueting Cao,Lingshen Meng,Jianxiang Wu,Xuejing Yang,Yefei Li,Zhipan Liu,Ming Gong
The paired electrolysis via anodic organic oxidation and cathodic hydrogen evolution has been an emerging hydrogen production technology with high efficiency and high values. Nickel oxyhydroxide is a special electrocatalyst that is capable of selectively oxidizing various alcohols, aldehydes, and amines to the corresponding carboxylates and nitriles at more favorable potentials compared to the oxygen evolution reaction. However, its detailed molecular-level mechanism is still in debate, especially for the potential-dependent behavior of some organic substrates. In this study, we revealed that the nickel oxyhydroxide can be dissected into two functional regions with a more facilely oxidized surface for facilitated substrate adsorption and a relatively inert bulk phase for accelerated electron transfer via probe-assisted kinetics and in situ surface-enhanced Raman spectroscopy. The prerequisite of the two regions conceals a universal potential-dependent oxidation behavior for almost all organic substrates. Further combining with the computational investigation unravels the origin of this potential dependence from the exothermic O/N-centered adsorption process on the surface and the rate-limiting proton-coupled electron-transfer (PCET) steps for the C–H bond breaking that demands bulk electron conductivity. This provides a rationale for designing more conductive underlayers to break the intrinsic limitations of nickel oxyhydroxide toward more efficient organic electrooxidation processes.
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JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Zixiao Qin,Jian He,Yin Zhu,Xiaopeng Wei,Jilin Wang,Guoyuan Zheng,Shuyi Mo,Bing Zhou,Fei Long
A new type of large-size two-dimensional organic-inorganic hybrid single crystal (C 7 H 10 N) 2 MnCl 4 was synthesized by the solvent evaporation method. The single crystal diffraction test and the method of analysis show that the crystal belongs to the Cc spatial group to the monoclinic system. And through Hirshfeld surface analysis and two-dimensional fingerprint analysis of the interaction between molecules in the single crystal growth process, it is known that the crystals mainly interact through hydrogen bonds. The absorption in the purple band was better, and its optical band gap value E g = 4.47 eV, which belongs to the wide band gap perovskite material. Based on thermogravimetric analysis, the crystal presented, good thermal stability, and its initial decomposition temperature is 185°C. Finally, the impedance spectrum of ingle crystal was studied, and the relaxation activation energy E a = 0.46927 eV was obtained by Arrhenius formula fitting according to the relationship between frequency and temperature. The temperature rises and the change law of the number of carriers, the changes of AC conductivity and DC conductivity by frequency and temperature are studied. The AC conductivity shows that the material has the potential of impedance sensors.
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Journal of Energy Chemistry
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2023
·
IF 13.1
Qiqi Mao,Wenxin Wang,Kai Deng,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts . Herein, we reported a low-content Pt-doped Rh metallene (Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen (H 2 ) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization. Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of −10 mA cm −2 in the hydrogen evolution reaction (HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm −2 in the hydrazine oxidation reaction (HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage (0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm −2 for energy-saving H 2 production, which greatly reduces the electrolysis energy consumption. Moreover, DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d -band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.
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MOLECULES
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2023
·Vol. 28
·期 13
·5021
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IF 4.6
Xinlan Han,Jinhua Li,Siyu Tao,Guowei Dou,Sanawar Mansur,Xinqian Zhang
The specific structure and diverse properties of hybrid organic–inorganic perovskite materials make them suitable for use in photovoltaic and sensing fields. In this study, environmentally stable organic–inorganic hybrid perovskite luminescent materials using Pb–MOF as a particular lead source were prepared using a mechanochemical method. Based on the fluorescence intensity of the MAPbBr3/MOF composite, the mechanized chemical preparation conditions of Pb–MOF were optimized using response surface methodology. Then, the morphological characteristics of the MAPbBr3/MOF composite at different stages were analyzed using electron microscopy to explore its transformation and growth process. Furthermore, the composite form of MAPbBr3with Pb–MOF was studied using XRD and XPS, and the approximate content of MAPbBr3in the composite material was calculated. Benefiting from the increase in reaction sites generated from the crush of Pb–MOF during mechanical grinding, more MAPbBr3was generated with a particle size of approximately 5.2 nm, although the morphology of the composite was significantly different from the initial Pb–MOF. Optimal performance of MAPbBr3/MOF was obtained from Pb–MOF prepared under solvent-free conditions, with a milling time of 30 min, milling frequency of 30 Hz and ball–material of 35:1. It was also confirmed that the mechanochemical method had a good universality in preparing organic–inorganic hybrid perovskite/MOF composites.Keywords:Pb–MOF;organic–inorganic hybrid perovskite/MOF composites;mechanochemical method;optical properties
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ACS Catalysis
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2022
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IF 13.7
Tian-Yu Qiu,Ying-Nan Zhao,Wen-Si Tang,Hua-Qiao Tan,Hui-Ying Sun,Zhen-Hui Kang,Xia Zhao,Yang-Guang Li
To conveniently regulate photocatalytic reactions, the design and development of smart photocatalysts, which can realize a series of controllable regulation of their structure, physicochemical properties, photocatalytic activity, and selectivity by simple external stimuli, such as chemical substances, pH, light, electric field, and heat, has aroused keen interest. However, the relevant research is still in its infancy. Herein, a smart imine covalent-organic-framework (COF) photocatalyst HP-n (n represents the pH of COF pretreatment, n = 1∼7) with proton-initiated switchable photocatalytic aerobic oxidation has been prepared. In the structure, the imine units can be reversibly protonated, which leads to the COF skeleton rearrangement from the phenolic to its quinone structure. The corresponding absorption band edge is expanded from 463 nm (HP-7) to 630 nm (HP-1). Meanwhile, the excitation energy transfer, oxygen adsorption, and activation change significantly, endowing HP-n with smartly switchable 1O2 production and interesting proton-initiated efficiency photocatalytic sulfide oxidation with both conversion and sulfoxide selectivity >99%. This work demonstrates a smart imine-COF photocatalyst, which paves the way for the development of smart photocatalysts and reveals the critical roles of protons in the structure–property–activity relationship of COF photocatalysts.
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ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Guangli He,Yunhe Lai,Yanzhen Guo,Hang Yin,Binbin Chang,Man Liu,Shouren Zhang,Baocheng Yang,Jianfang Wang
Designing plasmonic photocatalysts with spatially controlled catalytic sites is an effective strategy to boost the sunlight-driven chemical transformation efficiency through plasmonic enhancement. Herein, we describe a facile method for the synthesis of TiO2-tipped Au nanobipyramids (NBPs) to give (Au NBP)/t-TiO2 nanodumbbells. The surfactant cetyltrimethylammonium bromide concentration is the key factor in the construction of this type of unique nanostructure. The photocatalytic aerobic oxidative coupling of amines using the plasmonic photocatalysts with the dumbbell-like and core@shell structures indicates that the TiO2-tipped ends for the photo-reduction and the exposed adjacent Au surface for the photo-oxidation on (Au NBP)/t-TiO2 can significantly improve the photocatalytic activity. The underlying mechanism of the photocatalytic oxidative coupling of benzylamine over (Au NBP)/t-TiO2 has been thoroughly investigated. Both experimental and simulation results for (Au NBP)/t-TiO2 and (Au nanorod)/t-TiO2 confirm the important effect of the plasmonic hotspots on the enhancement of the photocatalytic activity.
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Sustainable Energy & Fuels
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2022
·Vol. 6
·期 23
·5261-5267
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IF 6.813
Ke Guo,Guang'an Jie,Jiahui Liu,Yanghe Fu,Rui Ma,Xinqing Lu,Fumin Zhang,Weidong Zhu,Maohong Fan
Photocatalytic selective oxidation in organic synthesis has been emerging as an environmentally friendly and energy sustainable approach to produce valuable chemicals, yet it remains a great challenge. In this study, a vanadium(IV) metal–organic framework constructed from triphenyl-based organic linkers, named BIT-66, was first employed as a photocatalyst for the selective oxidation of amines and sulfides in the presence of molecular oxygen or tert-butyl hydroperoxide (TBHP). BIT-66 possesses efficient visible-light absorption and photoinduced charge generation properties, and exhibits an excellent photocatalytic performance for oxidation reactions to produce valuable imines or sulfoxides with a high selectivity under visible light, as well as good reusability. The reactive oxygen species were further investigated via lots of quenching experiments and electron paramagnetic resonance trapping measurements for photocatalytic reactions. It is found that the superoxide radicals, resulting from the photogenerated electron transfer of the excited BIT-66, could be the main active species in the oxidative coupling of amines, while both hydroxyl and peroxyl radicals together play crucial roles in the oxygenation of sulfides using TBHP as the oxidant. This study demonstrates the great potential of photoactive MOFs for organic transformations to produce valuable chemicals.
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