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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

In-Sn alloy core-shell nanoparticles: In-doped SnOx shell enables high stability and activity towards selective formate production from electrochemical reduction of CO2

Jigang Wang,Shunlian Ning,Mi Luo,Dong Xiang,Wei Chen,Xiongwu Kang,Zheng Jiang,Shaowei Chen

SnO 2 has been recognized as excellent catalyst towards formate production from electrochemical CO 2 reduction (CO 2 R). However, it is a great challenge to prepare SnO 2 that is stable under the working condition of CO 2 R and the active center of the SnO 2 -based catalyst towards CO 2 R has been illusive. In this work, Sn-In alloy nanoparticles display an InSn 4 intermetallic core and an amorphous In-doped tin oxide shell and a CO 2 -to-formate faradaic efficiency of 94% and a current density of 236 mA cm −2 was achieved at −0.98 V. Operando X-ray absorption and Raman spectroscopy reveal that the In-doped tin oxide shell remains stable under CO 2 R condition. Density functional theory calculations indicate that the In-doped tin oxide results in the formation of oxygen vacancy, stabilized tin oxide shell and exergonic pathway for CO 2 -to-formate, which might account for the high performance of the catalysts towards CO 2 R.

研究领域: 材料科学 · 电化学 · 催化 · 可持续能源
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY · 2021 ·Vol. 96 ·期 8 ·2238-2248 · IF 3.174

Highly efficient conversion of glucose to methyl lactate over hierarchical bimetal-doped Beta zeolite catalysts

Xiao-Yang Yue,Hui-Fang Ren,Chengming Wu,Jun Xu,Jifan Li,Chun-Ling Liu,Wen-Sheng Dong

BACKGROUND Methyl lactate is widely applied in the chemical, food, cosmetics and pharmaceutical industries. The conversion of carbohydrates over heterogeneous catalysts to methyl lactate is a promising environmentally benign process. RESULTS Hierarchical Sn-Beta zeolite (Sn-Beta) and corresponding bimetal-doped Beta zeolites (M-Sn-Beta; M = Zn, In, La, Ga, Ni) were prepared via a novel modified hydrothermal synthesis method to convert carbohydrates into methyl lactate. The introduction of Zn into Sn-Beta considerably improved the yield of methyl lactate from glucose, while for the catalysts containing In, La, Ga and Ni, such improvements were not observed. CONCLUSIONS A methyl lactate yield reaching up to 66.7% was obtained over Zn-Sn-Beta at 220 °C for 6 h. The enhanced catalytic performance was attributed to high Lewis acid density and strength, together with synergistic effects between framework Sn 4+ and Zn 2+ ions of Zn-Sn-Beta. Additionally, Zn-Sn-Beta demonstrated fructose and sucrose conversion into methyl lactate with yields of 68.4% and 70.0%, respectively. The Zn-Sn-Beta catalyst could be re-used at least five times with only a slight loss of methyl lactate yield. © 2021 Society of Chemical Industry (SCI).

研究领域: 化学工程 · 催化科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Synthesis of bifunctional tin-based silica–carbon catalysts, Sn/KIT-1/C, with tunable acid sites for the catalytic transformation of glucose into 5-hydroxymethylfurfural

Armin Rezayan,Ke Wang,Renfeng Nie,Tianliang Lu,Jianshe Wang,Yongsheng Zhang,Chunbao Charles Xu

Catalytic transformation of carbohydrates to bio-chemicals such as 5-Hydroxymethylfurfural (HMF) has become a hot research topic, but development of cost-effective/efficient catalysts and processes remains a challenge for industrial application. In this study, efficient bifunctional Sn/KIT-1/C catalysts with controllable acid sites were synthesized and applied for glucose-to-HMF conversion. Strong Lewis acid sites were introduced into the framework of disordered mesoporous silica by liquid-phase grafting of tin chloride, and Bronsted acid sites were generated by inserting carbon into the mesopores, followed by controlled oxidation of the carbon. Characterizations revealed that optimizing the amount of carbon source, and carbonization and oxidation temperature provided a proper amount and strength of acidity that could significantly catalyze glucose dehydration reaction to HMF with suppressed byproducts formation. The best catalyst Sn/KIT-1/C(75–400-300) demonstrated superior catalytic performance at 175 °C for 2 h under THF/H 2 O biphasic system, obtaining 78.4 ± 2.1% and 82.9 ± 2.4% HMF yield and selectivity, respectively. The high activity may be attributed to catalyst high surface area/porosity, and the presence of well-balanced amounts and strength of Lewis/Bronsted acid sites. The catalyst could maintain its excellent catalytic activity for five consecutive runs, suggesting the high physical–chemical stability of the catalyst. The results obtained in this work demonstrated that bifunctional metal-supported silica–carbon composites can be a promising catalyst for simple/complex carbohydrates conversion to HMF/bio-based chemicals.

研究领域: 催化 · 化学工程 · 材料科学 · 生物化学
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ACS Biomaterials Science & Engineering · 2019 · IF 4.511

Microporous Coatings of PEKK/SN Composites Integration with PEKK Exhibiting Antibacterial and Osteogenic Activity, and Promotion of Osseointegration for Bone Substitutes

Han Wu,Lili Yang,Jun Qian,Deqing Wang,Yongkang Pan,Xuehong Wang,Saha Nabanita,Tingting Tang,Jun Zhao,Jie Wei

To improve the antibacterial and osteogenic activities of poly(etherketoneketone) (PEKK), concentrated sulfuric acid (H2SO4) suspension with silicon nitride (SN) microparticle was utilized to modify PEKK surface. Through sulfonation reaction, microporous coatings of PEKK/SN composites were created on PEKK surface, which were integrated with PEKK substrate. The results showed that the content of SN in the microporous coatings increased with the increase of SN content in H2SO4 suspension (PKS without SN, PKSC5 and PKSC10 with 5 and 10 wt % SN content in H2SO4) and that the surface roughness and hydrophilicity of microporous coatings on PEKK were significantly improved with the SN content increasing. In addition, the microporous coating of PKSC10 with high SN content exhibited excellent antibacterial activity due to the synergistic action of the presence of amino (−NH2) and sulfonic acid (−SO3H) groups as well as the improvement of protein absorption. Moreover, the microporous coating of PKSC10 obviously stimulated adhesion, proliferation, and osteogenic differentiation of rat bone mesenchymal stem cells. Furthermore, histological and push-out load evaluation indicated that the microporous coating of PKSC10 significantly promoted osteogenesis and osseointegration in vivo. The results suggested that the microporous coating of PKSC10 with high SN content display good biocompatibility, antibacterial and osteogenic activities, and osseointegration ability, which would have great potential for bone substitutes.

研究领域: 材料科学 · 生物材料 · 生物医学工程 · 组织工程
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FUEL · 2023 · IF 7.4

Pore-engineering-dependence and hydrophobicity-dependence on stannosilicate zeolite catalyst for efficient Baeyer-Villiger oxidation

Jiaxing Zhang,Songcheng Bo,Weiping Liao,Kaixuan Yang,Ting Su,Hongying Lü,Zhiguo Zhu

As robust heterogeneous catalysts, stannosilicate zeolites (in particular Sn-Beta) exhibit excellent catalytic performance in aqueous Baeyer-Villiger oxidation due to their unique activation ability of carbonyl group. For a specific Sn-containing zeolite, pore-engineering and hydrophobicity are generally two coupled factors to impact catalytic behavior. How to distinguish the function of each factor in this selective oxidation is still a pending question. Bearing this in mind, five stannosilicate zeolites (Sn-MFI, Sn-MWW, Sn-Beta, Sn-MCM-41, and Sn-Y) were prepared to establish the relationship between the structure (Lewis acidity, pore-engineering, and hydrophobicity) and catalytic performance. Particularly, hierarchical Sn-Y zeolite was post-synthesized by a simple solid-state ion-exchange method, where Sn 4+ ions were incorporated into zeolite framework via reacting with silanol nests derived from dealumination process. In comparison with other stannosilicate zeolites, the obtained Sn-Y possessed excellent catalytic activity in Baeyer-Villiger oxidation irrespective of using aqueous hydrogen peroxide or bulky tert -butyl hydroperoxide as the oxidant. Structure-performance relationship revealed that Lewis acid site was the catalytically active center and the catalytic activity was depended on zeolite pore-engineering and hydrophobicity in aqueous B-V oxidation system. The relatively high catalytic activity of Sn-Y zeolite was ascribed to its excellent hydrophobicity and opened channel system. The former can be further enhanced by silanization treatment. Finally, the recyclability and deactivation mechanism were given insight. This work is aimed to provide some guidance for elaborately designing efficient stannosilicate zeolite catalyst for Baeyer-Villiger oxidation by precisely modulating pore-engineering and hydrophobicity.

CAS / MDL: 112-40-3 16415-12-6
研究领域: 催化 · 材料科学 · 化学工程 · 无机化学
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Cell Metabolism · 2022 · IF 31.373

Discovery of a potent allosteric activator of DGKQ that ameliorates obesity-induced insulin resistance via the sn-1,2-DAG-PKCε signaling axis

Zu-Guo Zheng,Yin-Yue Xu,Wen-Ping Liu,Yang Zhang,Chong Zhang,Han-Ling Liu,Xiao-Yu Zhang,Run-Zhou Liu,Yi-Ping Zhang,Meng-Ying Shi,Hua Yang,Ping Li

Summary sn-1,2-diacylglycerol (sn-1,2-DAG)-mediated activation of protein kinase Cε (PKCε) is a key pathway that is responsible for obesity-related lipid metabolism disorders, which induces hepatic insulin resistance and type 2 diabetes. No small molecules have been previously reported to ameliorate these diseases through this pathway. Here, we screened and identified the phytochemical atractylenolide II (AT II) that reduces the hepatic sn-1,2-DAG levels, deactivates PKCε activity, and improves obesity-induced hyperlipidemia, hepatosteatosis, and insulin resistance. Furthermore, using the ABPP strategy, the diacylglycerol kinase family member DGKQ was identified as a direct target of AT II. AT II may act on a novel drug-binding pocket in the CRD and PH domains of DGKQ to thereby allosterically regulate its kinase activity. Moreover, AT II also increases weight loss by activating DGKQ-AMPK-PGC1α-UCP-1 signaling in adipose tissue. These findings suggest that AT II is a promising lead compound to improve obesity-induced insulin resistance.

CAS / MDL: 3483-12-3 57-13-6
研究领域: 药理学 · 代谢 · 内分泌学 · 分子生物学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2022 ·Vol. 29 ·期 11 ·15337-15346 · IF 5.19

Preparation and evaluation of Pd-Sn modified Ru-Ir electrode for denitrification of high chlorine ammonia–nitrogen wastewater

Yang Zhen-xing,Shang Jie,Yan Guang-xu,Wang Yu-xian,Guo Shao-hui

In this paper, Pd-Sn modified Ru-Ir electrode was prepared by thermal oxidation method, and the effects of doping amount of Pd-Sn and synthesis conditions on Pd-Sn modified Ru-Ir electrode performance were studied. Linear sweep voltammetry(LSV), cyclic voltammetry(CV), and the Tafel curve were used to study the electrochemical performance of the Pd-Sn modified Ru-Ir electrode materials. The effects of the doping amount of Pd-Sn on the microstructure and valence states of Pd-Sn modified Ru-Ir electrode materials were investigated by SEM, TEM, XRD, and XPS. When the mass of Pd-Sn accounted for 1.5% of the total mass of the elements, the molar ratio of Ru-Ir was 2:1, and the molar ratio of Pd-Sn was 3:1; the LSV, CV, and the Tafel curves indicated that Pd-Sn modified Ru-Ir electrode had the lowest chlorine evolution potential (1.0640 V vs. SCE), the best CV curve coincidence, and the smallest corrosion current density (6.5 × 10 −4 A/cm 2 ), showing the best chlorine evolution performance, the best durability, and corrosion resistance; the characterization of SEM, TEM, XRD, and XPS showed that Pd-Sn was successfully doped into Ru-Ir electrode materials; the crystallinity of Pd-Sn modified Ru-Ir electrode was the highest, and the binding energy was the lowest, but the crystal form of Ru-Ir solid solution did not have changed. The optimal synthesis conditions of Pd-Sn modified Ru-Ir electrode material were as follows: Pd-Sn molar ratio was 3:1, calcination temperature was 500 ℃, calcination time was 4 h, and water was used as solvent. Pd-Sn modified Ru-Ir electrode can efficiently treat high chlorine ammonia–nitrogen wastewater, when the reaction volume was 200 mL, the initial concentration of NH 3 -N was 100 mg/L, the concentration of chloride ion was 5000 mg/L, the current was 0.75 A, and the reaction time was 40 min; the removal rate of ammonia nitrogen can reach 100%. Responsible editor: Weiming Zhang.

研究领域: 环境科学 · 电化学 · 材料科学 · 废水处理
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LANGMUIR · 2022 · IF 4.331

Tin Porphyrin-Based Nanozymes with Unprecedented Superoxide Dismutase-Mimicking Activities

Ling Li,Huan Li,Lin Shi,Lili Shi,Tao Li

As the oxidative stress is related to human aging and many diseases, a diversity of antioxidant biomimetic enzymes to eliminate reactive oxygen species in vivo and maintain the redox balance has attracted intensive attention. Of particular interest are superoxide dismutase (SOD)-mimicking artificial enzymes that bear inherent characteristics of natural counterparts but overcome their deficiencies in thermal and acidic stability. Inspired by the metallized active center of natural SODs, here, we engineered different groups of metalloporphyrins and found that Sn-metallized porphyrins can act as novel SOD mimics, in which Sn-metallized meso-tetra(4-carboxyphenyl) porphine (Sn-TCPP) can more effectively catalyze the disproportionation of superoxide radical anions (•O2–) into hydrogen peroxide and oxygen. Especially, Sn-TCPP-based metal–organic frame nanozyme (Sn-PCN222) displays an unusually high catalytic activity that remarkably exceeds those of commonly used counterparts. Such unprecedented catalytic behaviors are proposed to depend on the Sn(IV)/Sn(II) transition at the center of Sn-TCPP. In addition, the metal–organic framework (MOF) nanozymes also display higher thermal and acidic stability than natural SODs. Interestingly, we find that Sn-complexed methylated tetra-(4-aminophenyl) porphyrin shows an aggregation-induced SOD activity in an acidic environment, whereas conventional SOD mimics do not function well in this case. Given these unique features, our reported Sn-porphyrin-based nanozymes would be potent alternatives for natural SODs to be widely used in clinical treatments of oxidative stress-related diseases.

CAS / MDL: 553-12-8
研究领域: 生物化学 · 医学 · 材料科学
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Advanced Energy Materials · 2024 ·Vol. 14 ·期 26 ·2401114 · IF 24.4

Unlocking the Myths of Molecular Bonding State in Modulating Oxidation and Anderson Localization for Inorganic Sn/Pb-based Perovskite Solar Cells

Qin Li,Junjie Ma,Xuanchen Xu,Peng Gao,Meng Cai,Mengqi Han,Jing Yang,Yiqiang Zhang,Yanlin Song

The improvement of photovoltaic and stability performance of tin (Sn)-based halide perovskite solar cells is impeded by notorious oxidation issues and Anderson localization. Despite previous implements in antioxidation through the incorporation of Lewis base additives, there still exist ongoing uncertainties surrounding its complex interaction mechanisms. A perplexing phenomenon regarding accelerated oxidation in acrylic acid is discovered that deviates from conventional Lewis base–acid reaction. The underlying insights into the deprotonation of acrylic acid followed by the formation of a “tripod” ionic bonding form are provided, which results in amplifying the delocalization effect of electrons of Sn 2+ . Furthermore, with the assistance of acrylamide and acrolein, synergistic enhancement in terms of the antioxidation and suppression of Anderson localization can be achieved — a concept referred to as “Dual Synergistic Engineering”. This suppresses the oxidation of Sn 2+ and reduces Sn 4+ content by ≈76%. Meanwhile, the diffusion length is prolonged significantly from 195.9 to 458.9 nm. The optimized all-inorganic Sn/Pb-based perovskite solar cells exhibit a power conversion efficiency of above 14% with enhanced stability. These findings provide an alternative viewpoint for comprehending the impact of chemical interaction on oxidation and crystal growth in Sn/Pb-based perovskites.

研究领域: 材料科学 · 光伏技术 · 钙钛矿太阳能电池 · 固体物理 · 化学键合 · 半导体材料
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BIOTECHNOLOGY LETTERS · 2019 ·Vol. 41 ·期 6 ·789-799 · IF 2.154

Biocatalytic synthesis and characterization of sn-1/3 and sn-2 monoacylglycerols

Wang Xiuwen,Cheng Yang,Jin Qingzhe,Wei Wei,Wang Xingguo

Objectives To investigate the lipase-catalyzed synthesis of high purity sn -1/3 and sn -2 monoacylglycerols (1/3-MAG and 2-MAG) of different fatty acids (FAs). Results The 1/3-MAGs of three FAs (16:0, 17:0, 16:1) were synthesized using lipase-catalyzed esterification of glycerol with FAs. The 2-MAGs were obtained from the ethanolysis of synthetic triacylglycerols using sn -1,3 regiospecific lipase. The effects of lipase types, substrate ratio, temperature, reaction time and lipase load on the MAG conversion were studied. Under the optimal conditions, high purities (96.74%, 95.44%, 92.96%) with acceptable isolated yields (51.00%, 54.28%, 46.00%) were obtained for 1/3-16:0-MAG, 1/3-17:0-MAG, and 1/3-16:1-MAG, respectively. For 2-16:0-MAG, 2-17:0-MAG, and 2-16:1-MAG, the purities were 92.64, 95.04, and 96.48%, with isolated yields of 50.64, 52.16, and 26.12%, respectively. The molecular structures of the synthetic compounds were confirmed by 1 H NMR, and MS and the melting points were characterized by DSC. Conclusions High purity MAG isomers can be synthesized via lipase-catalyzed reactions to be building blocks for production of functional lipids, the melting points of which are largely governed by the hydrophobic interactions among the alkanyl chains.

CAS / MDL: 506-12-7 75-65-0
研究领域: 食品科学 · 生物化学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2026 · IF 4.5

Accelerated synthesis of Sn-Beta with high Sn content by tuning crystallization temperature

Xiaomei Yang,Mengqing Wang,Ziqing Huang,Lipeng Zhou

The crystallization temperature was investigated for the hydrothermal synthesis of Sn-Beta. The crystallization curves of Sn-Beta at different temperature were performed and the crystal growth activation energy was obtained. The synthesized samples, especially the fully crystallized Sn-Beta, were characterized by XRD, SEM, ICP, UV-vis DRS, XPS, FT-IR spectroscopy of framework vibration and pyridine adsorption. The results indicate that the crystallization time shortened from 7 days to 1 day for Sn-Beta with n Si / n Sn of 100 when the crystallization temperature was increased from 140 °C to 180 °C. But no crystal was obtained as the crystallization temperature was higher than 180 °C. The catalytic performance of the fully crystallized Sn-Beta obtained at different crystallization temperature was slightly different in the conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) and the conversion of glucose to methyl lactate due to the slight difference in silanol defects. Sn-Beta with n Si / n Sn of 80 can also be successfully synthesized after crystallization at 160 °C for 3 d, which shows much higher activity and selectivity than Sn-Beta with n Si / n Sn of 100 for the conversion of EL in high concentration (1.6 mol L −1 ) to GVL.

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Device · 2024 · IF 0

Europium redox doping to suppress Sn-I defect pairs in Sn perovskite photovoltaics

Xue Ma,Bin Zhao,Pengfei Guo,Yalan Zhang,Jianheng Zhou,Lang Liu,Yu Zhang,Yuanyuan Zhou,Ning Wang

Preventing the formation of Sn-I defect pairs is of vital importance for the fabrication of stable and efficient Sn perovskite solar cells (PSCs). This has spurred intensive efforts, which leave a formidable challenge of simultaneously addressing the unfavored chemical activities of Sn 2+ and I − in Sn perovskites. Herein, we report a europium (Eu) redox-doping method that leverages the facile reactions between Eu 2+ , Sn 4+ , and I 0 in the acidic environment of perovskite solution and thus alleviates the Sn-I defect pair issue. Experimental and theoretical investigations suggest that Eu 2+ could enter Sn perovskite lattice, altering the geometric and electronic structures of [SnI 6 ] 4− octahedra. This could reduce the energy barrier for charge transfer along the inorganic framework. Sn-PSCs with Eu redox doping deliver power conversion efficiencies up to 13.66% and improved stabilities.

研究领域: 材料科学 · 化学 · 能源技术
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