ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Jing Wang,Jianfeng Zhang,Shan Ni,Huifang Xing,Qiyu Meng,Yangyang Bian,Zihao Xu,Meng Rong,Huizhou Liu,Liangrong Yang
Highly selective capture of cesium (Cs+) from complex aqueous solutions has become increasingly important owing to its (133Cs) indispensable role in some cutting-edge technologies and the environmental mobility of radioactive nuclide (137Cs) from nuclear wastewater. Herein, we report the development of cation-intercalated lamellar MoS2 as an effective Cs+ adsorbent with the advantages of facile synthesis and highly tunable layer spacing. Two types of cations, including Na+ and NH4+, were employed for the intercalations between adjacent layers of MoS2. The results demonstrated that the adsorption capacity of the NH4+-intercalated material (M-NH4+, 134 mg/g) for Cs+ clearly outperformed the others due to higher loading percentages of cations and larger layer spacing. The cesium partition coefficients for M-NH4+ in the presence of 100-fold competing ions all exceed 1 × 103 mL/g. A simulated complex aqueous solution containing 15.37 mg/L Cs+ and highly excess of competing ions Li+, Na+, K+, Mg2+, and Ca2+ (20–306 times higher) was introduced to prove the practical application potential using our best-performing M-NH4+, showing a good to excellent partition ability of Cs+ among other cations, especially for Cs/K and Cs/Na with separation factors of 58 and 212, respectively. The adsorption and selectivity mechanisms were clearly elucidated using various advanced techniques, such as scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. These results revealed that the good selectivity for Cs+ can be ascribed to the differences in Lewis acidities, hydration energy, cation sizes, and in particular, the divergence of coordination modes which was successfully achieved after tuning the layer distance via the cation intercalation strategy. In addition, the material has fast kinetics (<30 min), wide range of pH tolerance (4–10), and good reusability. Overall, our studies point out that the tunable lamellar MoS2-based materials are promising adsorbents for Cs+ capture and separation.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Yimin Huang,Xueyan Li,Yan Peng,Hua Zhang,Anxian Shi,Xiujun Deng,Baoling Wang,Yingtang Zhou,Bing Wang,Guangzhi Hu
The discharge of hexavalent chromium [Cr(VI)] in industrial wastewater into the natural environment can seriously cause harm to the environment and human health. We modified chitosan (CS) with Co and polydopamine (PDA) to synthesize a spherical adsorbent (CS–Co/PDA HCl ) for Cr(VI) removal from wastewater. Co doping can help CS–Co/PDA HCl maintain a high adsorption capacity (666.7 mg g -1 ) for Cr (VI) while retaining a complete bead shape after multiple recycling. In addition, CS–Co/PDA HCl can maintain 96% of its initial adsorption capacity after five adsorption cycles, demonstrating a strong regeneration ability. Under competitive conditions, the adsorption capacity of CS–Co/PDA HCl for Cr(VI) greatly exceed its adsorption capacity for Ni (II) and Mn (II). Because of the high selectivity of CS–Co/PDA HCl for Cr(VI), 1 kg of CS–Co/PDA HCl (cost approximately $31) could reduce the concentration of Cr(VI) in 87 m 3 of secondary electroplating wastewater containing various complex components to the drinking water standard. Owing to the high selective adsorption capacity of CS–Co/PDA HCl for Cr(VI) and its good regeneration ability and expected economic feasibility, CS–Co/PDA HCl can find potential applications in removing Cr(VI) from real wastewater .
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Chi Ma,Wenlei Fan,Wei Qin,Yafei Guo,Lichun Ma,Nelson Belzile,Tianlong Deng
Although efficient removal of Cs from wastewater is of great importance because of the nuclear energy sustainable development and public health, removing cesium is challenging for the high concentrations of sodium and potassium ions coexist. In this work, we synthesized the first novel bismuth-doped layered tin sulfide (KBS) and applied it to the efficient green adsorption of liquid cesium resources. KBS could reach the adsorption equilibrium for Cs + within only 2 min with a theoretical adsorption capacity of 425.55 mg/g. Furthermore, the adsorption performance remained reliable after 10 cycles of use. The structure and properties of KBS were explained at the molecular level by DFT calculations, and the calculated results were in sound agreement with the experimental data. Meanwhile, in this study, the material was reinforced and shaped by the electrostatic interaction of Zein and sodium alginate hydrogel, and finally, Zein@SA/KBS spherical composite adsorbent was obtained. The problem of the difficult recovery of adsorbent and the secondary contamination was solved. The adsorption performance of Zein@SA/KBS on Cs + was better than most composite adsorbents and showed reliable stability. Therefore, the new microspherical adsorbent (Zein@SA/KBS) has great potential for industrial application in removing radioactive cesium from wastewater.
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LWT-FOOD SCIENCE AND TECHNOLOGY
·
2023
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IF 6
Yuan-song Zhang,Xuechao Xu,Juanli Yang,Mengyuan Tan,Wenyuan Zhou,Lu Gao,Zhen-quan Yang
Cronobacter sakazakii in powdered infant formula (PIF) can cause infections in newborns that are life-threatening. Establishing a High-performance evaluation method for C. sakazakii in the PIF is urgently needed. In this study, a chromogenic system based on phage-directed immobilized nanozyme for colorimetric measurement of C. sakazakii in PIF was constructed . Initially, our acquired phage EspYZU15 was electrostatically immobilized on the surface of a palladium-based nanozyme to produce EspYZU15 directionally immobilized Pd (EspYZU15@Pd). EspYZU15@Pd possesses outstanding peroxidase-like properties, catalyzing the chromogenic reaction of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H 2 O 2 . The ability of EspYZU15@Pd to recognize and trap host bacteria allows C. sakazakii to specifically inhibit the TMB chromogenic process catalyzed by EspYZU15@Pd. Based on this detection strategy, a visual quantification method for C. sakazakii ranging from 3.2 × 10 2 to 3.2 × 10 7 CFU mL −1 was developed, yielding a low limit of detection (LOD) of 3.6 × 10 1 CFU mL −1 . This method was able to successfully detect C. sakazakii in PIF, with outstanding recoveries ranging from 95.8% to 104.9%. These characteristics indicate that the EspYZU15@Pd-based chromogenic system has considerable promise for the colorimetric determination of C. sakazakii in PIF.
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JOURNAL OF LUMINESCENCE
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2023
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IF 3.6
Linhong Liao,Xiao Lin,Jie Zhang,Zhiyuan Hu,Fengshou Wu
The nitrogen-doped carbon dots ( N -CDs) with multicolor emission (green, yellow, and red) were fabricated with naphthalenetetracarboxylic dianhydride as carbon precursor, and different alkylamines as passive agents. The structures of the as-prepared carbon dots were confirmed by the Fourier transform infrared (FT-IR) spectrum, X-ray photoelectron spectroscopy (XPS) spectra , transmission electron microscopy (TEM), Raman spectra , and X-ray diffraction (XRD) pattern. The characterized results and UV–vis absorption spectrum demonstrated that the luminescence variations of different CDs were probably attributed to the difference of N -related states, oxygen-containing groups, and oxidation degree in the CDs structure. Moreover, the green emitting CDs (G-CDs) could be utilized as fluorescent probe for ascorbic acid (AA) detection with detection limit (LOD) of 5 μM. The yellow emitting CDs (Y-CDs) could be used to detect glutathione (GSH) in the range of 1–70 μM with LOD of 0.07 μM. The red emitting CDs (R-CDs) could detect the water content in THF , DMF, acetone, and EtOH with LODs of 0.44%, 0.31%, 0.55% and 0.55%, respectively. Remarkably, G-CDs and Y-CDs can distinguish AA and GSH respectively with high selectivity and accuracy. Finally, the fluorescent probes based on G-CDs and Y-CDs were successfully applied for the AA and GSH determination in vitamin C tablet, grapefruit juice, and GSH whitening serum samples with high reliability and feasibility, which provided the guidance for the selection of AA and GSH supplements.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Kailong Gao,Hongxia Guo,Yanan Hu,Hongbin He,Mowen Li,Xiaoming Gao,Feng Fu
The efficiency of photocatalytic overall water splitting was mainly limited by the slow reaction kinetics of water oxidation. How to design effective surface active site to overcome the slow water oxidation reaction was a major challenge. Here, we propose a strategy to accelerate surface water oxidation through the fabrication spatially separated double active sites. FeCoPi/Bi 4 NbO 8 Cl - OVs photocatalyst with spatially separated double active site was prepared by hydrogen reduction photoanode deposition method. Due to the high matching of the spatial loading positions of FeCoPi and OVs with the photogenerated charge distribution of Bi 4 NbO 8 Cl and corresponding reaction mechanisms of substrate, the FeCoPi and OVs on the (001) and (010) crystal planes of Bi 4 NbO 8 Cl photocatalyst provided surface active site for water oxidation reaction and electron shuttle reaction (Fe 3+ /Fe 2+ ), respectively. Under visible light irradiation, the evolution O 2 rate of FeCoPi/Bi 4 NbO 8 Cl OVs was 16.8 μmol h −1 , as 32.9 times as Bi 4 NbO 8 Cl. Furthermore, a hydrogen evolution co-catalyst PtRu@Cr 2 O 3 was prepared by sequential photodeposition method. Due to the introduction of Ru, the Schottky barrier between PbTiO 3 and Pt was effectively reduced, which promoted the transfer of photogenerated electrons to PtRu@Cr 2 O 3 thermodynamically, the evolution H 2 rate on PtRu@Cr 2 O 3 /PbTiO 3 increased to 664.8 times. On based of the synchronous enhancement of the water oxidation performance on FeCoPi/Bi 4 NbO 8 Cl-OVs and water reduction performance on PtRu@Cr 2 O 3 /PbTiO 3 , a novel Z - Scheme photocatalytic overall water splitting system (FeCoPi/Bi 4 NbO 8 Cl-OVs) mediated by Fe 3+ /Fe 2+ had successfully constructed. Under visible light irradiation, the evolution rates of H 2 and O 2 were 2.5 and 1.3 μmol h −1 , respectively. This work can provide some reference for the design of active site and the controllable synthesis of OVs spatial position. On the other hand, the hydrogen evolution co catalyst (PtRu@Cr 2 O 3 ) and the co catalyst FeCoPi for oxygen evolution contributed to the construction of an overall water splitting system.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Sen Yang,Yinghao Wei,Qi Wang,Zhijun Sun,Ai-Hua Li
Lead-free double perovskites have superb luminescence properties for broad applications. However, increasing or improving near-infrared (NIR) photoluminescence (PL) is still a challenge. In this paper, a high-performance microcrystal is designed based on Tm 3+ heavily doped Cs 2 Ag 0.6 Na 0.4 In 0.9 Bi 0.1 Cl 6 (CANIBC), which realize both the self-trapped excitons (STEs) and Tm 3+ NIR emission. The emission mechanism and energy transfer (ET) process are studied by steady-state and time-resolved PL spectra. The ET efficiency from STEs to Tm 3+ can reach 38.3 %, and the NIR PL quantum yield of Tm 3+ can reach 22.7 %. Meanwhile, the PL spectra of Tm 3+ -doped CANIBC microcrystals (MCs) with different concentrations are used to investigate their temperature sensing properties based on both fluorescence intensity ratio (FIR) and lifetime. Based on the FIR, relative sensitivity ( S r ) can reach 2.93 % K −1 at 303 K. Moreover, based on lifetimes, S r can maintain more than 1.55 % K −1 from 303 to 453 K, and maximum S r can also achieve 2.38 % K −1 at 360 K. These excellent luminescence and sensing properties offer greater development potential in the field of NIR phosphor and thermometry.
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Advanced Optical Materials
·
2023
·
IF 9
Yan Liu,Xing Dai,Xuelian Zeng,Xianrong Yuan,Yanan Wang,Yuhang Song,Haoyu Chen,Chao Zhang,Yong Wang,Li Wan,Yatao Zou,Weihua Ning,Baoquan Sun
Decreasing the power consumption of light-emitting diodes (LEDs) and increasing the energy generation of solar cells are crucial tasks toward the mitigation of greenhouse gas emissions and Paris Agreement goals. Lead (Pb)-free halide double perovskites, identified as environmentally friendly alternatives to Pb-based perovskites, are not deemed useful thus far due to the absence of high photoluminescence quantum yield (PLQY) examples and large bandgaps. Herein, penta-cationic antimony (Sb 5+ )-doping strategy is demonstrated for the benchmark material of Cs 2 NaInCl 6 , achieving blue emission with near-unity PLQY and the lowest bandgap of 1.24 eV. The excellent PLQY observed in the material is attributed to Sb 5+ doping-induced Jahn–Teller distortion in Cs 2 NaInCl 6 and a newly emerged band structure, which has remained undisclosed in all previous reports. This groundbreaking discovery represents the first instance in the field of perovskite materials where the incorporation of a single dopant has resulted in a zero-to-one enhancement in their emission profile. This breakthrough is expected to have profound implications for advancing research in the utilization of similar dopants, such as manganese cations (Mn 6+ and Mn 7+ ), not only in halide perovskite structures but also in oxide-based perovskites and other semiconductor systems.
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Advanced Optical Materials
·
2023
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IF 9
Linan Wang,Chenchen Tu,Jiazheng Zhou,Yu Chu,Zhihua Yang,Shilie Pan,Junjie Li
The development of anti-laser damage infrared (IR) nonlinear optical (NLO) materials is an urgent need but challenging due to the contradiction between wide bandgap and large NLO coefficient. Herein, by introducing a halogen into the NLO-active tetrahedral unit, two halogenated metal chalcogenides Cs 3 Ga 8 S 13 Cl and Cs 9 Ga 8 Se 12 Cl 9 with unprecedented [GaQ 3 Cl] (Q = S/Se) tetrahedral units are rationally designed and fabricated in experiments by the flux method, enriching the chemical and structural diversity of chalcogenides. Cs 3 Ga 8 S 13 Cl shows a wide bandgap of ≈3.76 eV, resulting in a high laser-induced damage threshold of ≈8 × AgGaS 2 (AGS) and a moderate NLO response (≈0.6 × AGS) with phase-matching behavior. The results imply that Cs 3 Ga 8 S 13 Cl is a promising IR NLO material for the high powder laser application and demonstrate the feasibility of the halogenated tetrahedron strategy in regulating the optical properties of chalcogenides.
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NANOTECHNOLOGY
·
2023
·Vol. 35
·期 11
·115203
·
IF 3.5
Qingyong Qin,Yu Liu,Ge Gao,Zhaoqiong Chen,Zejiang Gao,Li Chen,Xianci Zhong,Bingsuo Zou
Lead-free halide double perovskites are considered as one of the most promising materials in optoelectronic devices, such as solar cells, photodetectors, and light-emitting diodes (LEDs), due to their environmental friendliness and chemical stability. However, the extremely low photoluminescence quantum yield (PLQY) of self-trapped excitons (STEs) emission from lead-free halide double perovskites impedes their applications. Herein, Sb3+ ions were doped into rare-earth-based double perovskite Cs2NaScCl6 single crystals (SCs), resulting in a large enhancement of PLQY from 12.57% to 87.37%. Moreover, by co-doping Sb3+ and Ho3+ into Cs2NaScCl6 SCs, the emission color can be tuned from blue to red, due to an efficient energy transfer from STEs to Ho3+ ions. Finally, the synthesized sample was used in multicolor LED, which exhibited excellent stability and optical properties. This work not only provides a new strategy for improving the optical properties of Cs2NaScCl6 SCs, but also suggests its potential application in multicolor LEDs.
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MICROCHEMICAL JOURNAL
·
2023
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IF 4.8
Sisi He,Yiyi Liu,Chaoxian Chi,Dongdong Zhou,Chuan-Fan Ding,Xucong Lin,Jiabin Wang,Fangling Wu
The differentiation of 3-AminoPyrrolidine (3AP) and its derivative isomers is significant due to their use as intermediates in drug synthesis. However, the separation of these isomers, which exhibit both chiral and positional isomerism, has consistently posed challenges. In this study, an efficient analytical method was developed to discrimination between the four isomers of R/S-I/N-Boc-3-AminoPyrrolidine (R/S-l/N-Boc-3AP) and four groups of derived chiral isomers, namely R/S-N-Methyl-3-AminoPyrrolidine (R/S-N-Me-3AP), R/S-N-Ethyl-3-AminoPyrrolidine (R/S-N-Et-3AP), R/S-1-Bzl-3-AminoPyrrolidine (R/S-1-Bzl-3AP), and R/S-1-Cbz-3-AminoPyrrolidine (R/S-1-Cbz-3AP). The discrimination was achieved by utilizing natamycin (Nat) as a differentiation agent and 2/3/4-aminobenzenesulphonic acid (2/3/4-ABSA) as ligand. The facile discrimination of the four positional isomers of R/S-1-Boc-3AP and R/S-N-Boc-3AP was achieved using ion mobility spectrometry (IMS) based on their formed diastereomeric complexes [Nat + (Boc-3AP) 2 + (2-ABSA) 2 + H] + . The isomers were also studied via tandem mass spectrometry (MS/MS) using the formed ternary complexes, different fragment ions were observed for l-Boc-3AP and N-Boc-3AP, but the R/S enantiomers cannot be discriminated either. In addition, the enantiomers R/S-l-Bzl-3AP and R/S-l-Cbz-3AP were differentiated based on mobility using [Nat + (R/S-l-Bzl-3AP) + (3-ABSA) 2 + H] + and [Nat + (R/S-l-Cbz-3AP) + 2-ABSA + H] + ; however for the small enantiomeric molecules of R/S-N-Me-3AP and R/S-N-Et-3AP, chiral discrimination was not achieved via the ternary complexes of Nat + R/S-N-Me-3AP-ABSA and Nat + R/S-N-Et-3AP-ABSA. Importantly, the separation was greatly improved by the coordinated alkali metal ions, where the separation resolution (R p-p ) increased with the radius of the metal ions. Finally, quantitative analysis and method validation were carried out for the four Boc-3AP isomers using both MS/MS and IMS-MS. Overall, the proposed method opens possibilities for the rapid discrimination and quantification of isomers exhibiting both chiral and positional isomerism in MS/MS and IMS-MS analyses.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Qingqing Wu,Jiaorong Yan,Mingxiang Jiang,Qiguang Dai,Jinyan Wu,Minh Ngoc Ha,Qingping Ke,Xingyi Wang,Wangcheng Zhan
Two-dimensional γ-Al 2 O 3 nanosheet with rich pentacoordinate Al 3+ sites which can nicely stabilize noble metals via strong interactions between metal and support has been focused. However, the synthesis of ultrathin and highly thermal-stable Al 2 O 3 is challenging. Herein, we report an effective approach to synthesize ultrathin Al 2 O 3 nanosheets with regular leaf-like architecture as well as high thermal-stability. A novel intercalation-swelling-exfoliation pathway was proposed to elucidate the formation of ultrathin sheet-like structure and then its morphology/thickness could be further adjusted via a dissolution-growth induced by phosphate. Meanwhile, the presence of phosphate further enhanced thermal stability of Al 2 O 3 nanosheets due to the occupation or depletion of high-reactive sites and surface hydroxy groups. Subsequently, the thermally stable γ-Al 2 O 3 nanosheets with moderate anchoring sites was used as a support of Pd and investigated for catalytic combustion of propane. The Pd/Al 2 O 3 nanosheet exhibited a superior catalytic activity for propane combustion and the complete conversion was below 300 °C, more importantly, the outstanding resistance to high temperature (1000 °C) was observed, which was ascribed to the re-dispersion of Pd particles and the occurrence of strong metal-support interaction (SMSI) at high temperature.
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