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ANALYTICAL CHEMISTRY · 2022 · IF 8.008

Retrieving Spectra of Pure Components from the DOSY-NMR Experiment via a Comprehensive Approach Involving the 2D Asynchronous Spectrum, 2D Quotient Spectrum, and Genetic Algorithm Refinement

Anqi He,Lei Ni,Hui Fu,Xiu Zhang,Zhen-Qiang Yu,Jun Song,Limin Yang,Yizhuang Xu,Yukihiro Ozaki,Isao Noda

When diffusion coefficients of different components in a mixture are similar, NMR spectra of pure individual components are difficult to be obtained via a diffusion-ordered spectroscopy (DOSY) experiment. Two-dimensional correlation spectroscopy (2D-COS) is used to analyze the data from the DOSY experiment. Through the properties of the systematic absence of cross-peak (SACP) in the 2D asynchronous spectra, spectra of pure components can be obtained even if their diffusion coefficients are similar. However, fluctuations in peak-position and peak-width are often unavoidable in NMR spectra, which makes SACPs unrecognizable. To address the problem, a 2D quotient spectrum is used to identify the masked SACPs. However, undesirable interference peaks due to the fluctuations in peak-position and peak-width are still present when we extract a spectrum of a component by slicing the 2D asynchronous spectrum across the SACP. A genetic algorithm (GA) is used to select a suitable subset of spectra where the diversities of peak-position and peak-width are significantly reduced. Then, we used the selected spectra to construct a refined 2D asynchronous spectrum so that the spectra of pure components with significant attenuated interference can be obtained. The above approach has been proven to be effective on a model system and a real-world example, demonstrating that 2D-COS possesses a bright perspective in the analysis of the bilinear data from DOSY experiments.

CAS / MDL: 1634-04-4
研究领域: 分析化学 · 核磁共振波谱学 · 数据分析
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Journal of the Taiwan Institute of Chemical Engineers · 2025 · IF 6.3

An interfacial networked self-cleaning membrane based on 2D/2D C-g-C3N4/BiVO4 heterojunction for photocatalytic degradation of tetracycline

Yanhua Cui,Yixuan Hong,Weilong Shi,Zengkai Wang

Background Photocatalytic membrane technology has attracted widespread concern in the field of water purification due to its high-efficiency and eco-friendly. However, the active sites of photocatalyst are easily embedding in the polymer membrane, consequently reducing degradation efficiency of photocatalytic membrane. Methods In this study, two-dimensional/two-dimensional regenerated silk fibroin-carbonized carbon modified graphite carbon nitride/bismuth vanadate heterojunction (2D/2D C-g-C 3 N 4 /BiVO 4 ) with excellent photocatalytic performance was synthesized by electrostatic self-assembly method. Then C-g-C 3 N 4 /BiVO 4 heterojunction was selected as catalytic structural units, three-dimensional (3D) interfacial networked poly(vinylidene fluoride) membrane-supported C-g-C 3 N 4 /BiVO 4 heterojunction (C-g-C 3 N 4 /BiVO 4 /PVDF) was fabricated by electrospinning technique. The combination of C-g-C 3 N 4 /BiVO 4 heterojunction and interfacial networked PVDF membrane synergistically enhanced their permeability, antifouling and antibacterial performance. Significant findings The optimized C-g-C 3 N 4 /BiVO 4 /PVDF photocatalytic membrane had higher degradation TC efficiency (83.33 %) than other membrane samples, and the efficiency of bacterial inactivation of C-g-C 3 N 4 /BiVO 4 /PVDF could reach 99.00 %. The C-g-C 3 N 4 /BiVO 4 /PVDF exhibited tremendous enhancement in the permeability (13,488.2 L m −2 h −1 ) and flux recovery efficiency (94.44 %). The free radical trapping tests and ESR spectra indicated that superoxide radical (·O 2 ⁻ ) was the dominant active species. In addition, the as-prepared C-g-C 3 N 4 /BiVO 4 /PVDF could easily recover and reuse, and photocatalytic activity basically remain unchanged, highlighting the potential application of membrane photocatalyst for the practical wastewater treatment.

CAS / MDL: 25155-30-0
研究领域: 环境科学 · 材料科学
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ACS Applied Energy Materials · 2022 · IF 6.959

2D/2D/1D Structure of a Self-Supporting Electrocatalyst for Efficient Hydrogen Evolution

Jinping Zhang,Yingxue Li,Chunyan Xu,Jing Li,Liying Yang,Shougen Yin

MXene-based electrocatalysts for hydrogen production have been extensively studied. Herein, we report an efficient and stable electrocatalyst (TiVCTx/MoS2-CNT) with a 2D/2D/1D structure, which is used for electrocatalytic hydrogen evolution. The catalytic performance can be attributed to the rich inherent anchoring sites of TiVCTx, which contribute to the uniform growth of MoS2 nanosheets and reduce the aggregation of MoS2 nanosheets. In addition, multiwalled carbon nanotubes (MWCNTs) are connected to form a 3D nanohybrid, which increases the conductivity of TiVCTx/MoS2 and provides a pathway for the electron transfer of TiVCTx/MoS2. As expected, TiVCTx/MoS2-CNT presented impressive hydrogen evolution activity with an overpotential of 180 mV at 10 mA/cm2 and a small Tafel slope of 79 mV/dec. Furthermore, TiVCTx/MoS2-CNT catalysts exhibit an electrochemical durability of up to 17 h in 0.5 M H2SO4. This work may provide a new idea for the construction of a three-dimensional nanohybrid and the development of an advanced bimetallic MXene-based nanohybrid for the hydrogen evolution reaction (HER).

CAS / MDL: 12054-85-2
研究领域: 材料科学 · 电化学 · 能源科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Interfacial charge transfer in 0D/2D defect-rich heterostructures for efficient solar-driven CO2 reduction

Hainan Shi,Saran Long,Shen Hu,Jungang Hou,Wenjun Ni,Chunshan Song,Keyan Li,Gagik G. Gurzadyan,Xinwen Guo

Two-dimensional graphitic carbon nitride (g-C 3 N 4 ) has been widely explored as a promising photocatalyst for solar CO 2 conversion. However, rapid charge recombination and low visible-light utilization are severely detrimental to photocatalytic CO 2 conversion. Zero-dimensional/two-dimensional (0D/2D) heterostructures are considered the promising materials with size tunability and enhanced charge separation efficiency for photocatalysis. Herein, a 0D/2D heterostructure of oxygen vacancy-rich TiO 2 quantum dots confined in g-C 3 N 4 nanosheets (TiO 2- x /g-C 3 N 4 ) was prepared by in-situ pyrolysis of NH 2 -MIL-125 (Ti) and melamine. Charge dynamics analysis by time-resolved photoluminescence (tr-PL) and femtosecond and nanosecond pump-probed transient absorption (TA) spectra revealed that charges transfer occured from 2D-g-C 3 N 4 to 0D-TiO 2 at an ultrafast subpicosecond time scale (<1 ps) through the intimate interface. The overall fast decay of the charge carriers was attributed to interfacial charge transfer, which was accompanied by recombination relaxation mediated by shallow trapped sites. Ultrafast interfacial charge transfer greatly promoted charge separation and electrons in shallow trapped sites were easily trapped by CO 2 . In addition, combining with the synergetic advantage of strong visible light absorption, high CO 2 adsorption and large surface area, TiO 2- x /g-C 3 N 4 exhibited a superior CO evolution rate of 77.8 μmol g −1 h −1 , roughly 5 times that of pristine g-C 3 N 4 (15.1 μmol g −1 h −1 ). This work provides in-depth insights into optimizing the heterojunction for robust solar CO 2 conversion.

研究领域: 材料科学 · 环境科学 · 化学
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Nanomaterials · 2023 ·Vol. 13 ·期 1 ·202 · IF 5.3

Preparation of 2D ZIF-L and Its Antibacterial and Antifouling Properties

Jingyu Li,Yang Zhang,Haichao Zhao,Guoxin Sui

The excessively leached metal ions from traditional metallic antimicrobial nanoparticles are harmful to biological and human tissues. Metal-organic frameworks (MOFs) coordinating bioactive metal ions to organic bridging ligands can potentially address this issue, avoiding the excessive leaching of metal ions and simultaneously exhibiting high effective antibacterial activities. Here, we report the preparation of a 2-dimensional leaves-like zeolitic imidazolate framework (ZIF-L) for potential antibacterial and anti-algae applications. The ZIF-L nanosheet exhibits complete inactivation ofEscherichia coli(phosphate buffer saline: 4 h) andBacillus subtilis(seawater: 0.5 h). The ZIF-L/epoxy composite has excellent antibacterial effect, poisoning effect and anti-adhesion effect on a variety of marine algae. It is worth noting that the removal rate (Escherichia coli) for ZIF/epoxy composite can be reached to 90.20% by only adding ZIF-L (0.25 wt%). This work will inspire researchers to develop more metal-organic frameworks materials for applications in the antibacterial and anti-algae fields.Keywords:ZIF-L;two dimensional;antibacterial;anti-algae

CAS / MDL: 693-98-1 9046-10-0
研究领域: 材料科学 · 生物医学工程 · 环境科学
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

In-situ construction of 3D marigold-like CoAl-LDH/Ti3C2 heterosystem collaborating with 2D/2D interface for efficient photodegradation of multiple antibiotics

Tianyu Wang,Yong Yang,Qinghua Deng,Xiaoyue Zhang,Lijun Xiong,Zheng Tang,Panjie Li,Nan Yin,Aiwu Sun,Dan Chen,Jinyou Shen

Developing of a photocatalyst for multiple antibiotics degradation and revealing their different mechanism are of great importance for wastewater remediation. Herein, a 3D marigold-like CoAl-LDH/Ti 3 C 2 hybrid is developed via in situ growth of CoAl-LDH on Ti 3 C 2 nanosheets and on-spot self-assembly during the hydrothermal process. The existence of optimized Ti 3 C 2 steers the morphology evolution from 2D lotus leaf-like nanoplate to 3D marigold-like hierarchical architecture, which greatly boosts the adsorption capacity and photon capture of the catalyst by the increased specific surface area and the scattering cross section. Meanwhile, the well-defined 2D/2D interface between the components effectively promotes the electron transfer from CoAl-LDH to Ti 3 C 2 , and the photoinduced electron-hole pairs on CoAl-LDH can be greatly separated. The density functional theory (DFT) calculations further demonstrate the change of electronic structure for the composite photocatalyst. As a result, CoAl-LDH/Ti 3 C 2 hybrid presents 85%, 56% and 70% degradation efficiency towards tetracycline hydrochloride, chloramphenicol and terramycin, which are 3.1, 3 and 2.1 times of the pristine CoAl-LDH. Furthermore, the degradation path for chloramphenicol is explored and the reason for its different degradation efficiency is revealed. The design of 3D hierarchical scaffold cooperating with 2D/2D heterogeneous interface provides a new avenue to develop ideal catalysts for wastewater remediation.

研究领域: 环境科学 · 材料科学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2025 · IF 5.4

Synergetic promotional effect of dual oxygen vacancies and 2D/2D TiO2/BiOBr S-scheme heterostructure for boosted photocatalytic oxytetracycline removal

Ying Tian,Kunfeng Zhang,Haoran Zhao,Bo Peng,Jinxia Liang,Hongxia Chen,Runfeng Huang,Yuanyuan Wei,Hanyu Chen

Novel 2D/2D TiO 2 /BiOBr (TOB- x , x represented the molar ratio of TiO 2 /BiOBr) heterostructures with dual oxygen vacancies were fabricated via an in-situ hydrothermal approach. Owing to the construction of p-n heterostructure and strong interface interaction, a S-scheme charge transfer path was formed, which facilitated efficiency separation and transfer of charge and retained strong redox capacities of photoexcited electrons and holes. Simultaneously, the introduction of oxygen vacancies induced strong photoabsorption, improving the light harvesting capacity. The oxytetracycline (OTC) degradation efficiencies over TOB-0.05 and TOB-0.1 were significantly improved relative to those of single components. The TOB-0.1 photocatalyst displayed the best photocatalytic activity, which was 3.75 and 1.76 times higher those of TiO 2 -Vo and BiOBr-Vo, respectively. Furthermore, we also examined the effects of pH, ions, and water matrixes on OTC conversion of TOB-0.1, and investigated the photocatalytic degradation mechanism. This work provides a useful guideline for constructing high-efficiency photocatalysts for wastewater treatments by combining 2D/2D heterojunction and dual-defect engineering.

研究领域: 环境科学 · 材料科学
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2D Materials · 2021 ·Vol. 8 ·期 2 ·021003 · IF 7.103

Highly efficient photoluminescence of 2D perovskites enabled by dimensional increasing

Linlin Ma,Chao Wang,Ya Chu,Yurong Guo,Xia Feng,Zhenyi Yu,Haoyue Zhang,Guangjiu Zhao

Herein, we proposed a dimension-increasing regulation strategy to realize the dimensionality engineering of perovskite from two-dimensional (2D) nanoplates (NPs) to quasi-two-dimensional (Q-2D) nanocrystals (NCs), and successfully prepared 2D (PEA)2PbBr4 NPs (PEA (phenylethylammonium) = C8H9NH3), Q-2D (PEA)2CsPb2Br7 (1) and (PEA)2Cs2Pb3Br10 (2) NCs. The photoluminescence dynamics changes from 2D (PEA)2PbBr4 NPs to Q-2D (1), (2) NCs by performing the time-resolved nanosecond transient absorption (NTAS) measurement for our perovskites. Compared with 2D (PEA)2PbBr4 NPs, we discovered for the first time that the electronic spectral redshift is intrinsic property of Q-2D NCs, which is caused by excitons transition to higher dimensionality. And the photoluminescence quantum yields (PLQYs) of Q-2D (1), (2) NCs is effectively increased from 8.780% to 14.72%, 21.80%, respectively. This directly verifies that Q-2D (1) and (2) NCs have enhanced their interlayer energy transfer capabilities. Moreover, the photoluminescence mechanism of these perovskites is investigated by the NTAS and the time-resolved photoluminescence (TR-PL) spectroscopy. The photophysical process of Q-2D samples exhibits a highly efficient and single photoluminescence pathway. The photoluminescence comes from the radiation recombination of free excitons. The Q-2D samples also have excellent photostability and decay lifetime stability. Our findings advance the research of improving 2D perovskites photoluminescence, and highlight potential of Q-2D NCs for optoelectronic applications.

研究领域: 材料科学 · 光学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Two-dimensional/two-dimensional heterojunction-induced accelerated charge transfer for photocatalytic hydrogen evolution over Bi5O7Br/Ti3C2: Electronic directional transport

Fangxia Xie,Qing Xi,Houfen Li,Xuan Jian,Jianxin Liu,Xiaochao Zhang,Yawen Wang,Rui Li,Caimei Fan

Regulating electron density at the active site by electronic directional transport from special channels is an effective strategy to accelerate the reaction rate in photocatalytic water splitting. Here, a novel two dimensional/two dimensional (2D/2D) Bi 5 O 7 Br/Ti 3 C 2 heterojunction with special interfacial charge transfer channel was fabricated successfully via in-situ growth of Bi 5 O 7 Br on the surface of ultrathin Ti 3 C 2 by using a convenient hydrolysis method. The electrostatic attraction between Bi 3+ cations and electronegative Ti 3 C 2 ensures the construction of 2D/2D heterojunction and a strong intimate interface contact between Ti 3 C 2 and Bi 5 O 7 Br, which establishes an electronic transport channel, and shortens the charge transport distance, assuring excellent bulk-to-surface and interfacial charge transfer abilities. Meanwhile, X-ray photoemission spectroscopy (XPS) and density functional theory (DFT) calculation revealed that the local electron density at the Ti 3 C 2 active sites is remarkably increased because of the transfer of interfacial electrons from Bi 5 O 7 Br to Ti 3 C 2 , which is a key factor for enhancing the photocatalytic performance. Thus, the resultant Bi 5 O 7 Br/Ti 3 C 2 exhibits significant improvement on the performance of photocatalytic hydrogen evolution under visible light irradiation . The hydrogen evolution reaction rate obtained on the optimized Bi 5 O 7 Br/Ti 3 C 2 composite is 1.97 times higher than that of pristine Bi 5 O 7 Br. This work provides a new protocol for the construction of 2D/2D heterojunction photocatalytic systems and regulating electron density by electronic directional transporting.

研究领域: 材料科学 · 光催化
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NANOTECHNOLOGY · 2021 ·Vol. 33 ·期 10 ·105601 · IF 3.874

High-pressure vapor-solid transformation of 2D template to derive 2D Co–N–C electrocatalysts for oxygen reduction reaction

Li Lin,Xing Du,Junjie Wang,Hui Chen,Xuan He,Wei Fang,Yang Li,Zhen Chen,Lei Zhao

Two-dimensional (2D) cobalt zeolitic imidazolate frameworks (ZIF-67) have attracted significant research interests to synthesize cobalt and nitrogen co-doped carbon-based (Co–N–C) catalyst for oxygen reduction reaction (ORR). However, most of the current synthetic approaches of 2D ZIF-67 are energy-intensive, environmentally hazardous and low-yield. Herein, a feasible and efficient 'morphology-retaining method via a high-pressure vapor-solid reaction' are reported to synthesize 2D ZIF-67 nanosheets by using 2D cobalt carbonate hydroxide template. In the strategy, the high-pressure vapor caused by sublimation of 2-Melm and the pores formed from effusion of CO2 during transformation ensure the complete transformation from 2D template to 2D ZIF-67. The corresponding 2D Co–N–C catalyst exhibits comparable ORR electrocatalytic activity and better stability than Pt/C in alkaline media. The present method is expected to offer a feasible and universal way to efficiently synthesize 2D M–N–C catalysts.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 电化学 · 催化
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MOLECULES · 2019 ·Vol. 24 ·期 16 ·2972 · IF 3.06

SYSU-6, A New 2-D Aluminophosphate Zeolite Layer Precursor

Jiang-Zhen Qiu,Long-Fei Wang,Jiuxing Jiang

Two-dimensional aluminophosphate is an important precursor of phosphate-based zeolites; a new Sun Yat-sen University No. 6 (SYSU-6) with |Hada|2[Al2(HPO4)(PO4)2] has been synthesized in the hydrothermal synthesis with organic structure-directing agent (OSDA) ofN,N,3,5-tetramethyladamantan-1-amine. In this paper, SYSU-6 is characterized by single-crystal/powder X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray analysis, transmission electron microscopy, infrared and UV Raman spectroscopy, solid-state27Al,31P and13C magic angle spinning (MAS) NMR spectra, and elemental analysis. The single-crystal X-ray diffraction structure indicates that SYSU-6 crystallized in the space groupP21/n, with a = 8.4119(3), b = 36.9876(12), c = 12.5674(3), α = 90°, β = 108.6770(10)°, γ = 90°, V = 3704.3(2) Å3, Z = 4, R = 5.12%, for 8515 observed data (I > 2σ(I)). The structure has a new 4,12-ring layer framework topology linked by alternating AlO4and PO4tetrahedra. The organic molecules reside between the layers and are hydrogen-bonded to the inorganic framework. The new type of layer provides a greater opportunity to construct zeolite with novel topology.Keywords:aluminophosphate;2-D zeolite;SYSU-6

CAS / MDL: 7664-38-2
研究领域: 材料科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Mineralization and toxicity reduction of the benzophenone-1 using 2D/2D Cu2WS4/BiOCl Z-scheme system: Simultaneously improved visible-light absorption and charge transfer efficiency

Runren Jiang,Guanghua Lu,Matthew Nkoom,Zhenhua Yan,Donghai Wu,Jianchao Liu,Tianjian Dang

Developing excellent photocatalysts to mineralize pollutants and reduce toxicity is an urgent problem in current environment purification research. Here, we synthesized a novel 2D/2D Cu 2 WS 4 /BiOCl Z-scheme system by a facile solvent mixing method and characterized the samples by various analytical methods. Compared with 3D/2D, the close contact surface of the 2D/2D catalyst endows it with extremely fast charge transfer and a large number of active sites, a Z-scheme system process strong electronic interaction and efficient charge separation, resulting in the high photocatalytic performance of the 2D/2D Cu 2 WS 4 /BiOCl Z-scheme system. As expected, The 15% 2D/2D Z-scheme Cu 2 WS 4 /BiOCl possessed the highest rate constant 1.14 × 10 −1  min −1 in the degradation of benzophenone-1 (BP1), which are 8, 5 and 4 times greater than that of BiOCl (1.36 × 10 −2  min −1 ), Cu 2 WS 4 (2.27 × 10 −2  min −1 ) and 15% 3D/2D Cu 2 WS 4 /BiOCl (2.6 × 10 −2  min −1 ), respectively. Meanwhile, the practicability of Cu 2 WS 4 /BiOCl was studied by the influence of relevant real water matrix on photocatalytic degradation of BP1. In addition, the result of density functional theory calculations demonstrated that the 2D/2D Cu 2 WS 4 /BiOCl system has faster charge transferability and closer integration than that of the 3D/2D system, which further confirms that the close 2D interface is conducive to charge transfer at the interface. Nine potential degradation products were identified as intermediates, and extremely significant toxicity reduction during the degradation process was confirmed by an ECOSAR prediction and zebrafish acute toxicity test . Compared with gene expression, the hatching rate and survival rate of zebrafish embryo are more sensitive and considered to be better choices for toxicity assessment.

研究领域: 环境科学 · 材料科学 · 毒理学
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