MATERIALS CHEMISTRY AND PHYSICS
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2021
·
IF 4.094
Cao Cheng,Hongyan Zhang,Fan Li,Shuguo Yu,Yan Chen
In this study, a gas sensor based on TiO 2 /WO 3 ·H 2 O (TW) heterojunction with high sensitivity, excellent selectivity and long-term stability for ammonia (NH 3 ) detection was successfully prepared by hydrothermal method . Compared with WO 3 ·H 2 O and TiO 2 , TW heterojunction shows excellent selective to NH 3 and the response varies by 3 orders of magnitude to 500 ppm NH 3 at room temperature (RT, 25 ± 3 °C). The lowest response limit of TW is 0.5 ppm and the response/recovery time is 2.35 s/1.95 s. The main reason for improving the performance of TW heterojunction to NH 3 detection is that TiO 2 nanoparticles cause more oxygen free radicals on the surface of TW heterojunction, which can react with more NH 3 molecules to release more electrons. Therefore, heterojunction structure increases the electrons and reduces the width of electron depletion layer in TW gas sensor. In addition, TW heterojunction has small and uniform particle size which can provide more active sites for the reaction between NH 3 and oxygen free radicals to release more electrons. This work provides a heterojunction structure composed of TiO 2 and WO 3 ·H 2 O to effectively improve the performance of sensor for NH 3 detection at RT, which is beneficial to the development of high-performance gas sensors.
研究领域:
材料科学
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化学工程
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传感技术
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DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2019
·
IF 4.978
Huai Liu,Xuejuan Cao,Ting Wang,Junnan Wei,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Shijie Liu,Lu Lin
The conversion of concentrated 5-hydroxymethylfurfural (HMF) or fructose to 2,5-furandicarboxylic acid (FDCA), a renewable alternative to petroleum-derived terephthalate acid, is highly desirable but challenging for FDCA production in an industrial scale. In this contribution, DMSO/H 2 O mixture was demonstrated as an effective medium for the production of FDCA from high concentration of HMF or fructose. For example, FDCA yield up to 93% was achieved at 10 wt% HMF concentration in DMSO/H 2 O over commercially available Ru/C (2 equiv. NaHCO 3 , 130 °C, 4 MPa O 2 and 12 h). Furthermore, an overall FDCA yield of 65% was achieved from concentrated fructose (19 wt%) through a facile two-step process. Notably, it is so far the highest HMF or fructose concentration employed for FDCA formation. As compared to pure water or DMSO , DMSO/H 2 O mixed system is able to stabilize HMF in an alkaline environment, which allows the efficient oxidation of HMF at high concentrations.
研究领域:
生物化学
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可再生化学
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绿色化学
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DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Zhige Zhang,Guican Bi,Shenglong Zhang,Tao Tan,Jun Xie
The use of biogas as renewable raw material to produce syngas(H 2 /CO ≈ 2)suitable for direct synthesis of methanol has attracted wide attention, but designing promising catalysts with high activity and stability remains a challenge. The catalytic systems used for this process usually have the characteristics of poor stability and easy carbon deposition. Here, Based on the Ce redox cycle and the strong metal-support interaction (SMSI), we designed and synthesized a series of Ni catalysts (denoted as Ni/CeMgO x /BN) with BN interfacial constraints. The abundant oxygen vacancy of reaction-induced Ce redox cycle endows Ni/CeMgO x /BN with excellent carbon resistance, because the ability to activate CO 2 /H 2 O is significantly enhanced. The CO 2 /H 2 O activation and carbon elimination mechanism were comprehensively characterized by in situ H 2 -TPR/CO 2 /H 2 O-TPSR, in situ CH 4 -TPSR/CO 2 /H 2 O-TPO, and FTIR, etc. Ascribed to the appropriate basicity of CeMgO x , homogeneous Ni dispersion, and strong interaction between Ni ultra-small nano particles (NPs) and CeMgO x /BN, Ni/CeMgO x /BN exhibit higher CO 2 /H 2 O adsorption/activation, higher CH 4 activation/dissociation, compared with another samples, which facilitate the formation of active oxygen species and intermediate coke removal, thus enhance the resistance to coke deposition and sintering. At 750 °C, Ni/CeMgO x /BN exhibit satisfying catalytic activity (CH 4 /CO 2 conversation 92 %/52 %) and superior stability (100 h) with negligible deactivation rates.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Jiangyao Chen,Jiajing Yi,Weikun Zhu,Weina Zhang,Taicheng An
O2 and H2O influence the photocatalytic oxidation mechanism of gaseous monoaromatics, but still in an unclear manner, due to the lack of direct evidence. Tracing an oxygen atom from 16O2 and H218O to intermediates can clarify their roles. The low H218O content suppressed the formation of benzenedicarboxaldehydes during the oxidation of xylenes and 16O2 greatly affected the yield of total intermediates, while neither of them altered the percentage order of the products. Methylbenzaldehydes, methylbenzyl alcohols, and benzenedicarboxaldehydes possessed greater 16O percentage (≥69.49%), while higher 18O distribution was observed in methylbenzoic acids and phthalide (≥59.51%). Together with the interconversion results of the products revealed, 16O2 determined the transformation of xylenes initially to methylbenzaldehydes and then to methylbenzyl alcohols or benzenedicarboxaldehydes, while H218O mainly contributed to conversion of methylbenzaldehydes to methylbenzoic acids or phthalide. Further interaction sites of xylene and its products with H2O and O2 were confirmed by molecular dynamics calculations. The same roles of 16O2 and H218O in the degradation of toluene, ethylbenzene, 1,2,4-trimethylbenzene, and 1,3,5-trimethylbenzene were also verified. This is the first report that provides direct evidence for the roles of O2 and H2O in the photocatalytic oxidation mechanism of gaseous monoaromatics. These findings are helpful to achieve controllable product formation from the oxidation of monoaromatics and predict their migration process in the atmospheric environment.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Yuqi Zhang,Xiang Yu,Li Xing,Tingting Fan,Xinyi Lian,Shuhong Zhang,Zhou Chen,Xiaodong Yi
A facile method for the large-scale production of 4MoO 3 ·2NH 3 ·H 2 O (MAH) nanocrystal with tunable size and morphology is developed through an antisolvent crystallization approach. The introduction of hydroxyl groups during crystallization promotes the formation of oxygen vacancies on the MAH. Due to the high concentration of Mo 5+ centres, small nanosheet thickness, and sandwich-like crystal structure, MAH-20 exhibits an outstanding adsorption capability toward cationic dyes, with the maximum adsorption capacities up to 1169.2 mg·g −1 for methylene blue (MB) and 1452.8 mg·g −1 for rhodamine B (RhB), which are almost 10 times as that of MAH-0. An electrostatic adsorption mechanism is proposed to interpret the highly selective adsorption activity toward cationic dyes. Moreover, a fast and recyclable treatment and adsorbent regeneration are realized based on a continuous flow filtration device.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CELLULOSE
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2020
·Vol. 27
·期 16
·9311-9324
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IF 4.21
Wang Mengdie,Yu Tingting,Tan Ling,Li Wei,Wei Wei,Jiang Man,Liu Dongqi,Zhou Zuowan
Abstract Applications of cellulose nanocrystals (CNCs) in various fields of high value have been and are being widely studied. However, research about the fundamental preparation method has come to a standstill. This work aims to introduce a concept of progressive dissolution of cellulosic fibers and an eco-friendly way of preparing CNCs. By controlling TBAH concentration, the amphiphilicity and dissolving capability of TBAH/H 2 O can be regulated. Through a controlled partial dissolution of cellulose in the solvent, aqueous tetra-butylammonium hydroxide (TBAH), the fiber can be dissolved to make nanoscale particles (CNC suspensions). Polarized light microscopy provides a quantitative evaluation of the progress of dissolution, by which a processing window (43% TBAH/H 2 O, 30 min dissolution at room temperature) for preparing CNCs from cotton pulp has been determined. The multiscale cellulose products, including micron-scale, nanoscale, and well-dissolved products of cellulose, have been separated with the assistance of the derivatization process. There are interestingly homogeneous materials of cellulose I with a needle-like shape in the nanoscale products extracted. Furthermore, the cellulose raw materials can be extended from cotton pulp to wood pulp, bamboo pulp, straw pulp, and microcrystalline cellulose, indicating it to be a universal method. Analysis of XRD patterns of the raw and CNCs indicates that amorphous and less-crystalline cellulose can be precisely and controllably dissolved by the solvent, leaving CNCs. Graphical abstract
研究领域:
材料科学
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化学工程
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生物质资源利用
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Longfei Zhao,Xin Chen,Yuan Zhang,Zhupeng Ye,Yanwei Zeng
In this paper, controllable nucleation and growth of CdS nanodots on the (020)-featured WO 3 ·H 2 O nanoplates has been successfully accomplished to prepare CdS-WO 3 ·H 2 O heterojunction with high-quality interfacial contact through a slow release of Cd 2+ and S 2- from the gradual self-loop hydrolysis of cadmium acetate and thioacetamide. The chemical and structural characteristics of as-prepared samples before and after heat treatment are detailedly investigated by TG-DSC, XRD, Raman, XPS, FESEM and HRTEM, as well as their light absorption performance from UV-Vis DRS. The maximum average hydrogen production rate for CdS-WO 3 ·H 2 O reaches 2.15 mmol·g −1 ·h −1 under 300 W Xe lamp irradiation (λ > 420 nm) using lactic acid as sacrificial reagent, which is 8.27 and 2.72 times as much as CdS and CdS-WO 3 , respectively. According to band alignment, CdS-WO 3 ·H 2 O exhibits greater energy difference of Fermi level than CdS-WO 3 , and augmented photocatalytic performance should arise from efficient Z-scheme charge transfer mechanism under stronger built-in electric field, in which the conduction band electrons of WO 3 ·H 2 O and valence band holes of CdS are expected to effectively recombine at their interfacial zones, while the conduction band electrons of CdS and valence band holes of WO 3 ·H 2 O contribute to the reduction of H + and oxidation of lactic acid.
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2022
·
IF 3.119
Jinqiu Ma,Ziquan Wang,Dan Li,Lingzong Meng,Yafei Guo,Tianlong Deng,Shuaiqi Sun,Yong Ma
The solubilities in the ternary system KCl–CsCl–H2O at 348.15 K were studied with the isothermal dissolution equilibrium method. The phase diagram of the system at 348.15 K is composed of one invariant point, two unvariant curves, and two single-salt crystallizations for KCl and CsCl. A comparison of the diagrams of the system KCl–CsCl–H2O from 298.15 to 348.15 K shows that the solid solution forms at 298.15 K and disappears at 323.15 and 348.15 K. Combining Pitzer binary parameters of KCl and CsCl obtained from the literature and solubility data in the system CsCl–H2O, the temperature dependence equations for Pitzer mixing parameters (θK,Cs and φK,Cs,Cl) and dissolution equilibrium constants of CsCl were built on the basis of the Pitzer model. The model for the mixed system provides reasonable mineral solubility from 273.15 to 348.15 K. The assumption of no solid solution existence in the ternary system can be applied in parameter fitting and solubility calculation. The results on the phase diagrams and thermodynamic model of the system KCl–CsCl–H2O can supply basic thermodynamic data and theoretical references for CsCl separation from the brine containing KCl.
研究领域:
化学热力学
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无机化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Linjia Li,Yiran Zhang,Xiaochao Wang,Junfeng Lu,Jiaqi Feng,Shu Zhao,Wei Qiu,Zhen Huang,He Lin
Integrated carbon capture and utilization (ICCU) technology based on Ca-Ni-based dual-function materials (DFMs) is an important carbon reduction measure. However, the severe performance degradation of DFMs caused by H 2 O is a challenge for ICCU. This study aims to improve the H 2 O resistance of Ce-doped Ni-Ca-based DFMs by Mg-Y co-doping. After 10 cycles with H 2 O, the carbon capture capacity, methane yield, and methane production rate were maintained at 11 mmol/g, 10.5 mmol/g, and 121.18 μmol/g·min, respectively. Changing the water vapor content (0 ∼ 10 %) has little effect on its performance. Characterizations (XRD, TEM, XPS, H 2 -TPR, CO 2 -TPD, NH 3 -TPD, H 2 -TPSR, and in-situ DRIFTS) and experiments (carbonation and conversion by H 2 O experiments) revealed a directional induced hydrogen spillover mechanism: The strong interactions of Ni-Mg and Ni-Y reduce the particle size and inhibit agglomeration; meanwhile, H 2 O can activate the Y-doped Ni-based catalyst in the carbonation process, inducing hydrogen spillover into the methanation reaction path during the subsequent conversion process, where Mg-promoted generated formaldehyde species act as a vital intermediate. It provides a novel idea to enhance the H 2 O resistance of DMFs to achieve stable ICCU performances.
研究领域:
化学工程
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环境科学
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材料科学
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Wenzhao Wei,Donggang Wang,Haibin Sun,Fangyong Yu,Xue Guo,Qiangqiang Hu,Yurun Feng,Hongli He,Xin Kong
Medium-entropy BaZr 0.1 Ce 0.5 Y 0.2 Dy 0.2 O 3-δ (BZCYD) electrolytes with a configurational entropy of 1.22 R are prepared by doping Dy element into low-entropy BaZr 0.1 Ce 0.7 Y 0.2 O 3-δ ( BZCY, 0.80 R). The entropy increasing strategy makes dramatically contribution to the improved chemical stability against CO 2 and H 2 O, and the relevant mechanism is clarified by the density functional theory (DFT). The BZCYD electrolyte shows stable phase composition and micro-structure after CO 2 heat treatment at 700 °C for 3 h and H 2 O treatment boiled for 3 h, while generation of impurities of BaCO 3 and Ba(OH) 2 accompanied by destroyed micro-structure are formed in the BZCY electrolyte under the same conditions. The total conductivity decay rates of BZCYD electrolyte after CO 2 heat treatment and H 2 O treatment are 44.1 % and 52.5 %, respectively, which exhibit significantly better than those of BZCY electrolyte (88 % and 74 %). According to the first-principles calculation, BZCYD electrolyte has higher CO 2 reaction energy barrier (5.21 eV) and H 2 O reaction energy barrier (7.30 eV), as well as lower CO 2 adsorption energy (−5.182 eV) and H 2 O adsorption energy (−0.742 eV), so it has better chemical stability. The peak power density of the anode-supported single cell with BZCYD electrolyte is 510 mW cm −2 at 700 °C in humid H 2 .
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2021
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IF 5.706
Huansheng Tan,Shibo Ma,Xiaoyu Zhao,Yushi Li,Chen Zhao,Yujun Zhu
Bimetallic W a CeO x (a = 0.06, 0.12, 0.18, 0.24) catalysts were synthesized for selective catalytic reduction of NO x with NH 3 (NH 3 -SCR). The influences of W on structure, activity and surface properties were investigated by XRF, XRD, Raman, TEM, N 2 adsorption-desorption, H 2 -TPR, O 2 /NH 3 /SO 2 -TPD, XPS, and in-situ DRIFTS. The characterization results show that the W/Ce ratio has a great effect on the NH 3 -SCR activity. The different catalytic activities of W a CeO x are mainly attributed to the acidity change, especially the increase of B-acid content plays a major role in enhancing low temperature activity. W 0.18 CeO x exhibits excellent low-temperature NH 3 -SCR activity, SO 2 /H 2 O resistance and N 2 selectivity with a broad activity window (190–490 °C) with 5%H 2 O. Moreover, good activity window (235–460 °C) can be maintained even the catalyst treated with 5% H 2 O at 800 °C for 12 h, showing especial hydrothermal stability. Thus, it can be summarized that W 0.18 CeO x is regarded as outstanding catalyst for low-temperature NH 3 -SCR of NO.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Shangguan Wenchao,Liu Qing,Wang Ying,Sun Ning,Liu Yu,Zhao Rui,Li Yingxuan,Wang Chuanyi,Zhao Jincai
Achieving CO 2 reduction with H 2 O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO 2 to CO with the help of H 2 O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g −1 h −1 (~100% selectivity), ~2.5 times the rate during CO 2 reduction with H 2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H 2 O decomposition, which synchronously optimizes the rate-determining steps in the CO 2 reduction and H 2 O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O 2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO 2 reduction with H 2 O.
研究领域:
化学
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材料科学
·
环境科学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子