INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Yunlong Xu,Linlin Yang,Chunying Si,Shuoqi Zhang,Quanxing Zhang,Guixiang Zeng,Wei Jiang
Sn-beta zeolite is a promising catalyst for the direct synthesis of lactide from lactic acid; here, we clarify the relationship between its local structure and activity through the interplay of experiments and DFT calculations. The open sites (HO-Sn-(OSi)3 with adjacent Si–OH) play a key role in the high activity of Sn-beta zeolite, where the reaction rate significantly decreases from 0.2258 mmol min–1 gcat–1 to 0.0724 mmol min–1 gcat–1 if the open sites were masked with Na+. Density functional theory (DFT) calculations show that the decrease in reaction rate comes from the weaker interaction between substrate and the open Sn site by Na+ exchange, which leads to the significant increase in the Gibbs energy barrier from 34.0 kcal/mol to 57.2 kcal/mol (rate-determining step). Other activities of heteroatom M-beta zeolites (where M = Ti, Zr, Hf) were also investigated, where the open sites were found to be crucial for the high activity in the direct synthesis of lactide as well. The information provided by this work is valuable for precise design of efficient catalysts for the one-step synthesis of lactide.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Shiwei Wang,Tianhao Li,Yanle Li,Hongfeng Yin,Ziqi Tian,Hongbo Yu
Supported Pt nanoparticles (NPs) exhibit excellent activity for the selective oxidation of glycerol (GL) derived from biodiesel production to high-value dihydroxyacetone (DHA). However, their selectivity to DHA is not satisfactory due to the preferential oxidation of the primary −OH in GL. In this study, Pt@Sn-MFI with ∼4.0 nm Pt NPs and different Si/Sn ratios were synthesized by an in situ encapsulation strategy. The optimized Pt@Sn-MFI-80 catalyst presents a 74.8% selectivity to DHA with a GL conversion of 43.5% at 60 °C. Our experiments and density functional theory (DFT) calculations indicated that the excellent selectivity was ascribed to the synergistic effect between Pt and Sn-MFI. Sn-MFI turned Pt NPs into an electronic-poor state so that suppressed further oxidation of glyceraldehyde (GLD); then, Sn-MFI triggered isomerization of GLD to generate DHA. The core–shell structure not only guaranteed an intimate contact between Pt and Sn-MFI but also enhanced the stability of the active Pt NPs.
研究领域:
化学工程
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Xiaofeng Liu,Yuanyuan Sun,Hao Ren,Yan Lin,Mingbo Wu,Zhongtao Li
Electrochemically driven carbon–carbon coupling utilizing renewable electricity under ambient conditions has emerged as an innovative approach for synthesizing high-value chemicals, which still faces inherent challenges such as low conversion rates and poor selectivity. While electroreducing furfural to hydrofuroin can produce high-quality biofuel, its efficiency need to be promoted. Herein, Cu–Sn bimetallic catalyst has been developed with a conversion rate of furfural of >97% and hydrofuroin selectivity of >67% through equilibrium of the interfacial intermediate *H and *fur-CHOH, which exhibits the greatest state-of-the-art overall performance. Characterization and theoretical calculation reveal that Cu serves as the active site for generating *fur-CHOH, whose electron density can be decreased by introducing Sn, and results in a higher *fur-CHOH coverage and a lower energy barrier of dimerization. Moreover, adding Sn also enables sluggish *H formation to balance interfacial *fur-CHOH and *H, leading to reduced hydrogenation byproducts. The as-developed approach provides valuable insights for optimizing other C–C electrocoupling reactions for the synthesis of high-value chemicals.
研究领域:
化学
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Shuang Wang,Lipeng Zhou,Beibei Gao,Yunlai Su,Xiaomei Yang
Sn-Beta is a good solid Lewis acid catalyst. Seed-assisted hydrothermal synthesis is a popular method for its preparation. However, the mechanism of seeds in the crystallization process is not clear. Here, the role of seeds in the growth of crystal and the influence on the properties of the corresponding products were studied. The seeds and gel was characterized by XRD , SEM, FT-IR and TG. During the crystallization, it was observed that the seeds were partially dissolved and formed seed fragments in the initial stage. Then the seed fragments acted as the core of the crystals and promoted the crystallization process. Seeds greatly decreased the crystal size of the products as compared with the direct hydrothermal method in absence of seeds. The acidity and catalytic performance of Sn-Beta synthesized via seeds route are similar with those of none-seeds method.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2019
·Vol. 22
·期 2
·248-256
·
IF 3.382
Xiuxia Wang,Chengyan Liu,Junliang Chen,Lei Miao,Shaohai Wu,Xiaoyang Wang,Zhengchuan Xie,Wenjing Xu,Qiufeng Chen
Recently, Ag8SnSe6-based materials, belonging to the family of argyrodite compounds, have been considered as promising thermoelectric candidates due to their intrinsically ultralow lattice thermal conductivity. However, their thermoelectric properties have been rarely investigated because of the intrinsic low carrier concentration. In this work, polycrystalline Ag8SnSe6 bulk materials were successfully synthesized by a bottom-up method by using hydrothermally synthesized Ag8SnSe6 nanocrystals as the precursors. The carrier concentration and mobility of Ag8SnSe6 are successfully enhanced by introducing additional Sn, which should manipulate the self-defects and improve the crystallinity. Thanks to the synergistic optimization of crystal and composition engineering, a maximum ZT value of about 1.22 is achieved for Ag8Sn1.005Se6 at 715 K, which is about 11% higher than that of the pristine sample, and the average ZT is also improved from about 0.65 to about 0.87. This study indicates that crystal engineering and composition engineering play an important role in the thermoelectric properties of Ag8SnSe6 and may provide guidance to improve the thermoelectric performance of other argyrodite compounds.
研究领域:
材料科学
·
热电材料
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2025
·
IF 9.1
Yingfu Tian,Tianliang Lu,Hongjin Qu,Xiaomei Yang,Lipeng Zhou
Efficient conversion of ethyl levulinate (EL) in high concentration to γ-valerolactone (GVL) at moderate temperature via catalytic transfer hydrogenation strategy is highly desirable. In this work, hydrothermally synthesized Sn-β zeolite with high Sn content was employed as a catalyst to realize this aim. Fully crystallized Sn-β zeolite with high Sn content ( n Si / n Sn = 60) was successfully synthesized within 12 days using MgCl 2 as a promoter. The synthesized zeolites were characterized by XRD, SEM, UV-vis spectroscopy, FT-IR spectroscopy and XPS. The L acid density of Mg-Sn-β-60-12d increased to 90 μmol g −1 compared to Mg-Sn-β-100-7d (56 μmol g −1 ). 92% yield of GVL was achieved on Mg-Sn-β-60-12d using high concentration of EL (1.2 mol L –1 ) as reactant at 130 o C for 8 h. The performance of Mg-Sn-β is better than that of Sn-β with same n Si / n Sn . The reaction mechanism over Mg-Sn-β was discussed. In addition, Mg-Sn-β-60-12d showed excellent stability and reusability during five runs.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHARACTERIZATION
·
2020
·
IF 3.562
Zhi-Chao Meng,Li-Yin Gao,Zhi-Quan Liu
Electrodeposition of Sn within porous anodic aluminum oxide (AAO) template was used to synthesize Sn nanowires. Ag seed layer was sputtered upon AAO template firstly, then the Sn nanowires were electroplated upon the seed layer. After electrodeposition the Ag seed layer was removed and the AAO template was dissolved in order to obtain Sn nanowires finally. The diameter of Sn nanowires was about 200 nm, being consistent with the template pore size, while the length of nanowires had a linear growth rate of approximately 2.49 μm/min. X-ray diffraction (XRD) and electron diffraction revealed that individual Sn nanowire was single crystal without preferential growth direction. The surface of the nanowire was wrapped by a thin SnO film (~5 nm thick), as verified by transmission electron microscopy (TEM) observation and X-ray photoelectron spectrometer (XPS) analyses. The synthesized Sn nanowire powders had a dark brown color, which comes from the surface SnO layer. Through the differential scanning calorimetry (DSC) analysis, the melting point of Sn nanowires was determined as 231.73 °C, which is about 2.7% lower than the pure Sn particles. Fabrication of Sn nanosolders from Sn nanowires was tried using liquid bath melting method. It was found that Sn nanowires could convert into spheroidal nanosolder in liquid paraffin, which demonstrated a novel technology to fabricate nanosolders used for nanoscale interconnections.
研究领域:
材料科学
·
纳米技术
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHARACTERIZATION
·
2022
·
IF 4.537
Shuang Liu,Limin Ma,Cheng Zhen,Yishu Wang,Dan Li,Fu Guo
In advanced microelectronic packaging technology, the interfacial brittleness of Cu/Sn solder joints puts forward higher requirements for high-performance diffusion barriers. Cobalt–Phosphorus (Co-P) alloy coating becomes ideal candidates for its good wettability and diffusion resistance. In this work, for Co-P with different crystallinity , the barrier properties of electrodeposited Co-P coatings as well as the mechanical properties of Co-Sn intermetallic compounds (IMCs) at the Co-P/Sn-Ag interface were investigated. According to the XRD results, the crystallinity of the Co-P coating was directly related to the phosphorus (P) content, and Co-P were classified into three types: crystalline state, mixed state and amorphous state. The morphology, composition, phase characterization, and mechanical properties of the Co-Sn IMCs at the interface were investigated by SEM , EPMA , TEM , and nanoindentation methods, respectively. After 180 °C aging test for 120 h, the thickness of CoSn 3 generated at the interface of crystalline Co-4.2 at.% P/Sn-Ag was the smallest among a total of 18 Co-P coatings, where P content ranged from 0.9 at.% to 20.8 at.%, showing the best barrier properties. The hardness of (Co,Cu)Sn 3 at the amorphous Co-P/Sn-Ag interface was the lowest (3.2 GPa), which was only 47% of that of Ni 3 Sn 4 , exhibiting the lowest brittleness tendency. The mixed crystalline-amorphous Co-P could greatly improve the diffusion barrier properties while sacrificing a small degree of brittleness comparing to the amorphous coatings, and had the potential to become a general-purpose alloy coating. This work could provide a scientific basis for the selection of Co-P barrier layers with excellent barrier properties and mechanical properties leading to different application scenario in electronic packaging.
研究领域:
材料科学
·
微电子封装技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2020
·
IF 4.189
Boyi Wang,Shuqi Zheng,Yuxuan Chen,Yue Wu,Juan Li,Zhen Ji,Yuning Mu,Zhibo Wei,Qian Liang,Jingxuan Liang
How to further improve the thermoelectric performance in Cu3SbSe4-based materials after optimizing its carrier concentration is a difficult issue. The present study attempts to address the issue by investigating thermoelectric performance of Cu3SbSe4 after Sn and La codoping, and all the samples were obtained by using a microwave-assisted hydrothermal synthesis method followed with the spark plasma sintering (SPS) process. First, a series of Cu3Sb1–xSnxSe4 (x = 0–0.03) compounds have been synthesized, and the hole carrier concentration obviously increased with increasing the Sn content. In addition, La doping subsequently was employed to the Cu3Sb0.98Sn0.02Se4 sample to further increase its power factor by band flattening, resulting in a typical high power factor of 1156.5 μWm–1 K–2 and zT of 0.67 in Cu3Sb0.92Sn0.02La0.06Se4 at 623 K. Our study provides a novel methodology through regulating its carrier concentration and band structure for designing high thermoelectric performance Cu3SbSe4-based materials.
研究领域:
材料科学
·
物理学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2012
·Vol. 14
·期 9
·2506-2512
·
IF 6.32
Jianjian Wang,Jiawen Ren,Xiaohui Liu,Jinxu Xi,Qineng Xia,Yanhong Zu,Guanzhong Lu,Yanqin Wang
5-Hydroxymethylfurfural (HMF) is a very important intermediate in the fine chemical industry. This study aims to investigate the direct conversion of glucose or glucose-based carbohydrates, such as sucrose, cellobiose, inulin, starch and cellulose, to HMF by using a Sn-Mont catalyst. With the use of this catalyst, a HMF yield of 53.5% was achieved from glucose in a mono-phase medium of tetrahydrofuran (THF)/dimethylsulfoxide (DMSO) at 160 °C for 3 h. The success of one-step conversion of glucose to HMF is attributed to the Sn-Mont catalyst containing two types of acid sites, Lewis acid and Brønsted acid sites. The former one plays a crucial role in the isomerization of glucose to fructose and the latter one is active in the dehydration of generated fructose to HMF. Furthermore, Sn-Mont catalyst also demonstrated excellent activity in the conversion of disaccharides and polysaccharides and as high as 39.1% HMF was directly obtained from cellulose in a THF/H2O–NaCl bi-phasic system.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2017
·
IF 6.844
Chuande Huang,Yanyan Zhu,Xiaodong Wang,Xin Liu,Junhu Wang,Tao Zhang
A series of BaFe 1− x Sn x O 3− δ catalysts were prepared by sol-gel method and tested for N 2 O decomposition to shed light on the effect of B-site substitution on the catalytic behavior of perovskite catalysts. 119 Sn and 57 Fe Mössbauer results confirmed that the 5-fold coordinated Fe 3+ cations with one adjacent oxygen vacancy (Fe 3+ O 5 ) were the main active centers for N 2 O decomposition. Doping of Sn cations can significantly improve the percentage of Fe 3+ O 5 from 30% ( x = 0) to 68% ( x = 0.8). More importantly, the valence state of Fe could be gradually reduced due to weakening of Fe O bond with increasing the Sn content, which was attributed to the stronger force of Sn than Fe in Fe O Sn structure to draw the oxygen anion and expansion of unit cell volume. Such change of Fe chemical state favored the oxygen mobility of the catalyst, leading to reduction in activation energy for N 2 O decomposition from ca. 241 ( x = 0) to 178 kJ mol −1 ( x = 0.8). BaFe 0.2 Sn 0.8 O 3− δ catalyst exhibited the highest intrinsic rate of 1.49 s −1 (550 °C), nearly 4 times larger than that of BaFeO 3− δ (0.43 s −1 ).
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 7
·1457
·
IF 4.6
Fenfen Guo,Yuxuan Wang,Zhicheng Jiang,Youjing Tu,Ruikai Li,Xingyu Zhang,Aoyi Tang,Yuan Liang,Lishi Yan,Hu Luo,Shenggang Li,Lingzhao Kong
The catalytic production of lactic acid from carbohydrates was considered a green way to efficiently utilize renewable biomass resources. In this study, an easy post-synthesis method was used to prepare a Sn-Beta catalyst for the production of lactic acid from glucose at 180 °C, 2 MPa, and 30 min. With optimized reaction time, temperature, pressure, and the ratio of raw material to catalyst, the yield of lactic acid reached an astonishingly high level of 76.0%. In addition, the catalyst characterizations were performed in-depth, revealing the intrinsic relationship between catalyst performance and structure, proving that the 2 wt% Sn was uniformly dispersed in the skeleton of Beta zeolite, which significantly increased the density of Lewis acid. Thus, the enhanced isomerization and retro-aldol condensation processes over the Lewis acid sites led to the high yield of lactic acid. This catalytic system kept stable after five cycles at mild conditions, showing high potential for industrial biomass utilization.
研究领域:
生物化学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）