ANALYTICAL SCIENCES
·
2022
·Vol. 39
·期 1
·13-22
·
IF 1.967
Chen Xianli,Liu Yi,Zhong Ming,Yang Jiangyong,Lin Zhenming,Liang Yong
Sialic acid (SA), known as N -acetyl neuraminic acid, is a natural 9-carbomonosaccharide derivative. SA has been widely applied in the early diagnosis of diseases as therapeutic target. However, the abundance of SA is very low in biological samples, which is usually interfered by the similar molecules coexisting at high abundance. Combining the advantages of high selectivity and specificity of molecularly imprinted technology, high specific surface area of mesoporous materials and excellent optical properties of quantum dots, we chose Mn-doped ZnS quantum dots as signal elements, and sialic acid as the template molecule. KH-4-MAPB with recognition ability to SA was synthesized by one-step hydrothermal method using thiolene click reaction as functional monomer. Based on the principle of boron affinity, molecularly imprinted polymers with highly ordered mesoporous structure were prepared, and the structure and fluorescence properties of fluorescent molecularly imprinted polymers were studied. FT-IR, XRD, TEM and nitrogen adsorption–desorption experiments were used to characterize the structure and morphology of the molecularly imprinted polymers. The results showed that the prepared molecularly imprinted polymers had highly ordered mesoporous structure and a large number of imprinted holes, which ensured the specific selectivity of the molecularly imprinted polymers. The fluorescence properties of MIMPs were characterized and analyzed by fluorescence spectra, equilibrium adsorption kinetics experiments were conducted and imprinting properties were recorded under different pH. The above experimental results showed that the fluorescence quenching was successfully achieved when the template molecule SA was captured by the molecularly imprinted polymer. When the concentration of SA was 1.25–100 × 10 –2 g/L, the fluorescence quenching degree of MIMPs showed a fine linear relationship with SA. The correlation coefficient was 0.9946, and the detection equation was F 0 / F − 1 = 0.0215 [CSA] + 0.0241. MIMPs had a high recognition ability for SA, and the imprinting factor was 2.44. As a fluorescent sensor for SA, the response time of MIMPs was 20 min. When the buffer solution pH was 7, the imprinting factor was the largest. Under the best conditions, MIMPs revealed good selectivity and specificity for the fluorescence recognition of SA. MIMPS were also applied to the analysis of SA in real human serum samples with satisfactory results. Graphical abstract
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yuanzhi Luo,Pan Wang,Gaixia Zhang,Sisi Wu,Zhangsen Chen,Hariprasad Ranganathan,Shuhui Sun,Zhicong Shi
To realize highly efficient and stable hydrogen production at high current densities, more efforts are devoted to developing outstanding water-splitting electrocatalysts. Herein, through a facile hydrothermal-phosphorization method, Mn-doped Ni 2 P/Fe 2 P was rationally designed and prepared as a high-performance bifunctional electrocatalyst for alkaline freshwater/seawater splitting. In alkaline seawater (freshwater) electrolyte, it merely needs low overpotentials of 358 (3 3 5) and 470 (4 0 5) mV to reach 1000 mA cm −2 for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively. This electrocatalyst also shows excellent stability even at a high OER current density of 500 mA cm −2 for 200 h. Regarding the alkaline overall seawater splitting, Mn-doped Ni 2 P/Fe 2 P presents a low cell voltage of 2.02 V at 500 mA cm −2 and outstanding stability for 120 h at the same current. The X-ray absorption fine structure (XAFS) experimental analysis verifies that the Mn doping and Ni 2 P/Fe 2 P heterointerfaces can efficiently optimize the electrocatalyst’s electronic structure, leading to the improved intrinsic OER and HER activities. Meanwhile, the 3D nanoflower structure provides abundant exposed active sites, and the Mn doping and heterointerfaces can create more active sites. Besides, the high corrosion resistance resulting from nickel-iron phosphides makes the electrocatalyst become a good candidate for seawater splitting. This study provides a simple path to fabricate highly active and robust non-noble electrocatalysts for freshwater/seawater splitting at high current densities.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2022
·Vol. 33
·期 20
·16383-16395
·
IF 2.779
Zhao Taolin,Chang Liyao,Ji Rixin,Chen Shaokang,Jin Xiaoyu,Zheng Yingdi,Huang Xiyun,Shen Jiangang,Zhang Yuxia
Recently, all types of electrical equipment put forward increasing requirements on the energy density of secondary rechargeable batteries. The low specific capacity of cathode material is the primary factor that restricts the energy density of Li-ion batteries. Li-rich Mn-based cathode materials have the advantages of high specific capacity, high operating voltage, low cost, and environmental friendliness. However, they have the limitations of low first Coulombic efficiency and serious capacity/voltage attenuation. In this work, lithium polyacrylate (LiPAA) has been employed as a water-soluble binder in the electrode to develop a high-performance Li-rich Mn-based cathode. The effect of the LiPAA binder on voltage drop and electrochemical performance of Li[Li 0.2 Co 0.13 Ni 0.13 Mn 0.54 ]O 2 cathode has been examined to reveal the modification mechanism. The results show that carboxyl group (–COOH) in the LiPAA structure can form strong hydrogen bonds with the oxygen atoms in the active material, making the electrode components firmly bonded and thus maintaining the structural stability of the cathode upon cycling. Moreover, the LiPAA binder can effectively inhibit voltage drop of Li[Li 0.2 Co 0.13 Ni 0.13 Mn 0.54 ]O 2 . The discharge voltage of the electrode decreases by only 117 mV after 50 cycles. Green water-soluble LiPAA has broad prospective applications as a binder of electrode materials of secondary batteries.
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Advanced Optical Materials
·
2022
·Vol. 10
·期 18
·2200706
·
IF 10.05
Xuying Feng,Yuhang Sheng,Kewei Ma,Fangjian Xing,Cihui Liu,Xifeng Yang,Hongqiang Qian,Shude Zhang,Yunsong Di,Yushen Liu,Zhixing Gan
Traditional fluorescent anti-counterfeiting labels can be easily cloned due to the lack of sufficient security. Therefore, multilevel anti-counterfeiting techniques with higher security need to be constantly explored. This study reports a multilayer composite structure containing Mn doped CsPbCl 3 (Mn:CsPbCl 3 ) perovskite quantum dots (PQDs) layer and CsPbBr 3 PQDs layer. The encrypted information is patterned on the Mn:CsPbCl 3 PQDs layer with weak orange fluorescence, which is concealed by the brighter green fluorescence of CsPbBr 3 PQDs at the upper layer. Based on the well-separated photoluminescence (PL) peak positions, inverse PL temperature-dependences and distinct PL lifetimes of these two PQDs, the encrypted information can be read out by adding cut-off filter, heating and using ultrafast camera (UCA)/pulsed excitation (PE). This multilevel anti-counterfeiting label significantly increases the difficulties of imitation meanwhile no expensive equipment is required for the verification of authenticity. Moreover, two bits of binary numbers that can be represented by dual emissions of the Mn:CsPbCl 3 PQDs by changing the doping content, which significantly increases the information storage capacity, are also demonstrated.
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BIOORGANIC CHEMISTRY
·
2022
·
IF 5.307
Han Xu,Ninghua Fu,Jie Zheng,Muhammad Sohail,Xing Zhang
Metal-organic frameworks (MOFs), as advanced enzyme immobilization platforms for improving biocatalysis and protein biophysics, are rarely investigated as solid supports in the enzymatic synthesis of carbohydrate and derivatives, which can be attributed to the complex biochemical reaction mechanisms and the adverse interactions between the high polarity of substrate sugars, glycoenzymes and traditional MOFs. Here, we introduced divalent metal ion Mn 2+ into MOF to prepare bimetallic MOF microreactor that encapsulated N -acetylhexosamine 1-Kinase (NahK), a critical anomeric kinase involved in the enzymatic synthesis of sugar nucleotide. The introduced Mn ions not only adjusted the microstructure of MOFs, but also participated in the enzymatic catalysis as cofactor, thus facilitated the N -acetylglucosamine/ N -acetylgalactosamine (GlcNAc/GalNAc) phosphorylation. The Mn-doped [email protected] organic material (MOM), integrated with high catalytic activity, high stability, and high recoverability, solved the issues of immobilization related to glucokinase activity. These features significantly improved the operability and reduced the processing cost, assuring industrial application prospects for sugar nucleotides synthesis.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Li Li,Zhi Huang,Yanying Liu,Ziqi Zhu,Mingjun Xu,Wenxuan Wei,Qian Zhang,Junming Hong
Novel porous Mn-Fe nanocubes (p-MnFe NCs) with abundant oxygen vacancies, which derived from Mn-Fe prussian blue analogue, were fabricated for the first time through annealing at H 2 atmosphere. Among the different molar ratios of Mn/Fe, p-Mn 1 Fe 1 NCs possessed abundant oxygen vacancies and exhibited excellent performance for peroxymonosulfate (PMS) activation to effectively degrade bisphenol A (BPA). As a result, 100% BPA (20 mg/L) degradation efficiency can be achieved within 30 min in the p-Mn 1 Fe 1 NCs/PMS system. SO 4 •− , HO•, O 2 •− and 1 O 2 were confirmed as main reactive oxygen species during catalytic reaction. The exposed Mn and Fe sites on the surface of p-Mn 1 Fe 1 NCs were the main active sites for the generation of reactive radicals. For non-radical generation pathway, the generated 1 O 2 and O 2 •− mainly originated from the reaction between dissolved oxygen and surface oxygen vacancies, and parts of 1 O 2 originated from the formation of intermediate O 2 •− . Radical and non-radical pathways were proposed in the p-Mn 1 Fe 1 NCs/PMS system for insights into the mechanisms of BPA degradation. Finally, the possible degradation pathways were proposed via ultra-performance liquid chromatography quadrupole time-of-flight mass spectrometry (UPLC-TOF-Q-MS) analysis.
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CHEMOSPHERE
·
2021
·
IF 7.086
Cui Lai,Huchuan Yan,Dongbo Wang,Shiyu Liu,Xuerong Zhou,Xiaopei Li,Mingming Zhang,Ling Li,Yukui Fu,Fuhang Xu,Xiaofeng Yang,Xiuqin Huo
Peroxymonosulfate (PMS)-based advanced oxidation processes for wastewater treatment have received extensive attention in the past years. Here, a novel Mn, Ce co-modified g-C 3 N 4 (MnCe-CN) composite was successfully synthesized by one-step pyrolysis for activating PMS. The physical and chemical characterization of MnCe-CN/PMS was conducted, indicating that Mn and Ce were evenly distributed on g-C 3 N 4 and existed in the form of Mn-N structure and CeO 2 , respectively. The MnCe-CN/PMS system could effectively degrade pollutants such as acetaminophen (ACT), methylparaben (MeP), p -nitrophenol (PNP), and 2,4-dichlorophenol (2,4-DCP). Among them, 2,4-DCP could be rapidly degraded, reaching 100% within 30 min. The masking experiments and electrochemical testing results revealed that 2,4-DCP was degraded via superoxide radicals (O 2 ˙ˉ), singlet oxygen ( 1 O 2 ), and electron transfer path. The cyclic experiments and real water treatment experiments testified that the oxidative system had excellent stability and applicability. This study provides a facile synthetic method to fabricate bimetallic co-modified g-C 3 N 4 for the enhancement of PMS activation .
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高影响因子
CHEMICAL PHYSICS LETTERS
·
2021
·
IF 2.328
Guanfeng Tian,Youqing Wu,Shiyong Wu,Sheng Huang,Jinsheng Gao
In 2 O 3 , MnO/In 2 O 3 , and MgO/In 2 O 3 catalysts are synthesized by the co-precipitation method and investigated for CO 2 hydrogenation to methanol. The introduction of Mn and Mg oxides dramatically enhances the CO 2 adsorption capacity of In 2 O 3 . The changing trend of methanol selectivity is consistent with the CO 2 adsorption capacity. MnO/In 2 O 3 and MgO/In 2 O 3 catalysts show higher methanol selectivity compared with that of In 2 O 3 .
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RARE METALS
·
2023
·Vol. 43
·期 1
·148-163
·
IF 8.8
Xu Zhi-Hui,Sun Shi-Shuai,Li Xue-Lei,Zhang Zhi-Hui,Li Hai-Ying,Ruan Shuang-Ting,Yin Shou-Gen
The balancing of the electrochemical performance, mechanical stability, and processing technology for applying supercapacitors to flexible and wearable electronics continues to encounter severe challenges. Herein, we prepare Ni–Co–Mn hydroxide electrodes with a three-dimensional multichannel structure via a simple hydrothermal method. These are constructed using vertically contiguous nanosheets with a uniform thickness and rough surface. The electrodes can provide numerous electroactive sites and accelerate the transmission of electrolyte ions. The relationship between the structure and electrochemical performances is verified by experiments and theoretical calculations. Two-dimensional (2D) planar and one-dimensional (1D) fiber electrodes are prepared using a flexible carbon cloth (CC) and carbon fiber (CF), respectively, as substrates. The assembled quasi-solid-state flexible asymmetric supercapacitor (FASC) with a two-dimensional sandwich structure using NiCoMn–OH/CC as the electrode achieves a remarkable energy density of 73.8 Wh·kg −1 at a power density of 1.03 kW·kg −1 . The quasi-solid–state FASC with a 1D linear structure using NiCoMn–OH/CF as the electrode also attains a high energy density (12.9 Wh·kg −1 at a power density of 0.75 W·kg −1 ). Moreover, the electrochemical performances of the NiCoMn/CC//AC/CC and NiCoMn/CF//AC/CF FASCs are not disturbed at different bending angles (0°, 45°, 90°, 135° and 180°). This indicates the superior flexibility of the devices. We also assemble a self-powered energy-harvesting storage system by integrating FASCs and commercial solar cells to verify its practicability. It displays sustainable development potential for energy storage. Graphical abstract
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Crystals
·
2023
·Vol. 13
·期 11
·1587
·
IF 2.7
Yiyi Xiao,Hui Huang,Jinkun Guo,Mi Yan,Liyuan Wei,Yu Liu,Shiliang Huang,Rufang Peng,Bo Jin
Energetic complexes represent a crucial research direction for the design and synthesis of novel energetic materials. In this work, 2,6-diamino-3,5-dinitropyrazine-1-oxide (LLM-105), a significant explosive compound with exceptional comprehensive properties, was selected as the ligand for coordinating with various metal ions. Four novel energetic complexes, Ni(C4H3N6O5)2·DMF (1), Co(C4H3N6O5)2·2DMF (2), Mn(C4H3N6O5)3·3/2DMF (3), and Cu3(C4H2N6O5)3·3DMF (4) were successfully synthesized, and their crystal structures were identified by a single-crystal X-ray diffraction technique. The structural analyses illustrated that LLM-105 can form either a mononuclear metal complex after the deprotonation of one amino group or a trinuclear metal complex after the deprotonation of two amino groups. Compound1exhibits a planar quadrilateral geometry, while both compounds2and3display distorted octahedral configurations. Compound4has three metal centers and exhibits two coordination configurations of distorted tetragonal pyramid geometry and planar quadrilateral geometry. The detonation performances of compounds1–4were also theoretically calculated, revealing their favorable explosive properties. These findings emphasize the diverse coordination modes of LLM-105 and the structural variability and adjustability of its complexes, offering valuable insights for regulating both the structure and performance of the LLM-105 complex as well as researching its deprotonation.Keywords:energetic complexes;LLM-105 ligand;single-crystal structure;coordination modes
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhuolin Cui,Tingting Hu,Shuqing Yang,Yu Yang,Xueyan Liu,Tao Wang,Huizhi Chen,Chunlai Zeng,Ruizheng Liang,Yubin Zhou
Sonodynamic therapy (SDT) has attracted increasing attention owing to its superior tissue penetration compared with other therapies. However, the development of multifunctional sonosensitizers with imaging capability and high production efficiency of reactive oxygen species (ROS) is still a challenge for current sonodynamic cancer therapy. Herein, we report the design and preparation of amorphous 2D Mn-doped CoMo-layered double hydroxide (a-Mn-CoMo-LDH) nanosheets (NSs) through acid etching-induced crystalline-to-amorphous phase transformation as a highly active nano-agent for magnetic resonance imaging (MRI)-guided SDT. The a-Mn-CoMo-LDH NSs exhibit superior ROS production capacity compared with amorphous CoMo-LDH NSs (∼1.3 times) and crystalline Mn-CoMo-LDH NSs (∼3.9 times) under ultrasound (US) irradiation, which is ∼ 9.9 times of the previously reported TiO 2 sonosensitizer. The doped Mn 4+ in the a-Mn-CoMo-LDH NSs can not only decompose H 2 O 2 into O 2 to alleviate the hypoxia level in tumor microenvironment (TME), but also consume glutathione (GSH) to reduce its clearance of ROS, promoting the SDT performance synergistically. Importantly, the GSH consumption can partially reduce the Mn 4+ to Mn 2+ within the tumors, which can serve as an agent for T 1 -weighted MRI, thus endowing the a-Mn-CoMo-LDH NSs with excellent MRI capability. Therefore, the as-prepared a-Mn-CoMo-LDH NSs with polyethylene glycol modification can be used as an efficient nano-agent for MRI-guided SDT, which can effectively achieve apoptosis of cancer cells in vitro and eradication of tumors in vivo under US irradiation.
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高影响因子
ACS Applied Energy Materials
·
2023
·
IF 6.4
Yuqing Hu,Puhui Deng,Wenying Wang,Linping Zhang,Yu Hou
Element doping and collaboration with other cocatalysts are two vital strategies to improve the photoelectrochemical properties and overcome the drawbacks of CdS for better photocatalytic performance. In this work, a series of manganese cadmium sulfides (MnxCd1–xS) were obtained by a solvothermal method. When x is equal to or greater than 0.3, MnxCd1–xS is composed of Mn–Cd–S sosoloid and MnS. Among all these MnxCd1–xS products, the Mn0.5Cd0.5S sample showed the best photocatalytic hydrogen production (5.99 mmol g–1 h–1). To further elevate the hydrogen production rate of Mn0.5Cd0.5S, four kinds of Ni-POMs were coupled with it as cocatalysts, and all these composite photocatalysts displayed enhanced performance. The highest efficiency was observed for 15-Ni4–Mn0.5Cd0.5S, which is up to 36.58 mmol g–1 h–1. Various characterizations indicated that Ni4P2W18, Mn–Cd–S sosoloid and MnS in the 15-Ni4–Mn0.5Cd0.5S composite form a double type-II heterojunction, which facilitates the separation and transfer of photogenerated carriers.
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