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基于碳化钼材料CO_(2)加氢制备高附加值化学品的热催化研究进展
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作者 徐勇庆 杨玉瑶 +10 位作者 武孟娜 杨潇潇 别璇 张时语 李清海 张衍国 张宸伟 Robert EPrzekop Bogna Sztorch Dariusz Brzakaski 周会 《物理化学学报》 SCIE CAS CSCD 北大核心 2024年第4期26-51,共26页
CO_(2)加氢对于CO_(2)转化制备高附加值化学品和燃料以实现二氧化碳利用及能源储存至关重要。CO_(2)加氢包括甲烷化、逆水煤气变换、甲醇化和CO_(2)直接费托合成等。碳化钼,尤其是其二维材料,由于其低成本和良好的性能而备受关注。在CO_... CO_(2)加氢对于CO_(2)转化制备高附加值化学品和燃料以实现二氧化碳利用及能源储存至关重要。CO_(2)加氢包括甲烷化、逆水煤气变换、甲醇化和CO_(2)直接费托合成等。碳化钼,尤其是其二维材料,由于其低成本和良好的性能而备受关注。在CO_(2)加氢反应中,由于碳的渗入,导致晶格膨胀以及价电子增加,碳化钼基催化剂展现出了类似于贵金属催化剂的性质。碳化钼可以通过程序升温渗碳法、选择性蚀刻法、机械合金合成法、化学气相沉积法、原位热渗碳法以及溶液相合成法等来制备。到目前为止,学者已经对基于碳化钼的材料的CO_(2)转化进行大量研究,这些材料具有良好的CO_(2)转化活性和对目标产物的选择性。碳化钼材料的催化性能可以通过调节碳化钼中的C/Mo比、在碳化钼与负载金属之间建立强的金属-载体相互作用以及调整材料的界面结构来实现。然而,基于碳化钼的热催化CO_(2)转化仍处于初级阶段。本文综述基于碳化钼的热催化CO_(2)加氢制备高附加值化学品和燃料的研究进展,并分析其面临的挑战和机遇。 展开更多
关键词 CO_(2)加氢 碳化钼 热催化 异相催化 MXenes
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New possibility for PET plastic recycling by a tailored hydrolytic enzyme
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作者 Shijie Yu Qinghai Li +1 位作者 yanguo zhang Hui Zhou 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第2期163-165,共3页
Plastic waste puts a huge burden on the ecosystem due to the current lack of mature recycling technology.Poly(ethylene terephthalate)(PET)is one of the most produced plastics in the world.Enzymatic decomposition holds... Plastic waste puts a huge burden on the ecosystem due to the current lack of mature recycling technology.Poly(ethylene terephthalate)(PET)is one of the most produced plastics in the world.Enzymatic decomposition holds the promise of recovering monomers from PET plastic,and the monomers can be used to regenerate new PET products.However,there are still limitations in the activity and thermal stability of the existing PET hydrolases.The recent study by Lu et al.introduced a novel PET hydrolase via machine learning-aided engineering.The obtained PET hydrolase showed excellent activity and thermal stability in the hydrolysis of PET and is capable of directly degrading large amounts of postconsumer PET products.This approach provides an effective method for recycling PET waste and is expected to improve the current state of plastic pollution worldwide. 展开更多
关键词 Plastic waste Poly(ethylene terephthalate) HYDROLYSIS Machine learning Enzymatic depolymerization HYDROLASES
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Breaking the temperature limit of hydrothermal carbonization of lignocellulosic biomass by decoupling temperature and pressure 被引量:4
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作者 Shijie Yu Xiaoxiao Yang +2 位作者 Qinghai Li yanguo zhang Hui Zhou 《Green Energy & Environment》 SCIE EI CAS CSCD 2023年第4期1216-1227,共12页
Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption... Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption have limited the development of HTC technology. In conventional batch reactors, the temperature and pressure are typically coupled at saturated states. In this study, a decoupled temperature and pressure hydrothermal(DTPH) reaction system was developed to decrease the temperature of the HTC reaction of lignocellulosic biomass(rice straw and poplar leaves). The properties of hydrochars were analyzed by scanning electron microscopy(SEM), Fourier transform infrared(FTIR) spectroscopy, X-ray photoelectron spectroscopy(XPS), Raman spectroscopy, X-ray diffraction(XRD), thermogravimetric analyzer(TGA), etc. to propose the reaction mechanism. The results showed that the HTC reaction of lignocellulosic biomass could be realized at a low temperature of 200℃ in the DTPH process, breaking the temperature limit(230℃) in the conventional process. The DTPH method could break the barrier of the crystalline structure of cellulose in the lignocellulosic biomass with high cellulose content, realizing the carbonization of cellulose and hemicellulose with the dehydration, unsaturated bond formation, and aromatization. The produced hydrochar had an appearance of carbon microspheres, with high calorific values, abundant oxygen-containing functional groups, a certain degree of graphitization, and good thermal stability. Cellulose acts not only as a barrier to protect itself and hemicellulose from decomposition, but also as a key precursor for the formation of carbon microspheres. This study shows a promising method for synthesizing carbon materials from lignocellulosic biomass with a carbon-negative effect. 展开更多
关键词 BIOMASS LIGNOCELLULOSE Hydrothermal treatment Hydrochar Carbon materials
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Selective hydrodeoxygenation of guaiacol to cyclohexanol using activated hydrochar-supported Ru catalysts
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作者 Kaile Li Shijie Yu +2 位作者 Qinghai Li yanguo zhang Hui Zhou 《Frontiers of Chemical Science and Engineering》 SCIE EI CSCD 2024年第5期13-22,共10页
Lignin,an abundant aromatic polymer in nature,has received significant attention for its potential in the production of bio-oils and chemicals owing to increased resource availability and environmental issues.The hydr... Lignin,an abundant aromatic polymer in nature,has received significant attention for its potential in the production of bio-oils and chemicals owing to increased resource availability and environmental issues.The hydrodeoxygenation of guaiacol,a lignin-derived monomer,can produce cyclohexanol,a nylon precursor,in a carbon-negative and environmentally friendly manner.This study explored the porous properties and the effects of activation methods on the Ru-based catalyst supported by environmentally friendly and cost-effective hydrochar.Highly selective cleavage of C_(ary)-O bonds was achieved under mild conditions(160°C,0.2 MPa H_(2),and 4 h),and alkali activation further improved the catalytic activity.Various characterization methods revealedthat hydrothermal treatment and alkali activation relatively contributed to the excellent performance of the catalysts and influenced their porous structure and Ru dispersion.X-ray photoelectron spectroscopy results revealed an increased formation of metallic ruthenium,indicating the effective regulation of interaction between active sites and supports.This synergistic approach used in this study,involving the valorization of cellulose-derived hydrochar and the selective production of nylon precursors from lignin-derived guaiacol,indicated the comprehensive and sustainable utilization of biomass resources. 展开更多
关键词 hydrochar GUAIACOL CYCLOHEXANOL activation full-component utilization
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颗粒团聚对稀相气固流动脉动关联项的影响
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作者 冯蘅 李清海 +2 位作者 蒙爱红 张衍国 孔博 《过程工程学报》 CAS CSCD 北大核心 2019年第2期279-288,共10页
研究了颗粒团聚对描述稀相气固两相流的气固相宏观控制方程中待封闭气固脉动关联项的影响规律并建立关键待封闭项代数模型。根据气相速度脉动与固相浓度关联项(漂移速度)控制方程,将漂移速度表达为固相非均匀程度和气固平均滑移速度的... 研究了颗粒团聚对描述稀相气固两相流的气固相宏观控制方程中待封闭气固脉动关联项的影响规律并建立关键待封闭项代数模型。根据气相速度脉动与固相浓度关联项(漂移速度)控制方程,将漂移速度表达为固相非均匀程度和气固平均滑移速度的代数模型。分别采用两种基于颗粒动理学的欧拉-欧拉框架介尺度方法模拟三维周期条件且固相平均浓度为1%的稀相气固两相流动,第1种方法假设固相速度分布函数f为各项同性的双流体方法(TFM);第2种方法假设f服从各向异性高斯分布的积分矩法(AG)。网格分辨率为颗粒直径dp的1.75倍,气固间动量交换采用Stokes曳力模型,并与文献中采用相同参数设置的欧拉-拉格朗日(E-L)方法模拟结果进行对比。结果表明,AG方法的准确度优于TFM方法,气固平均滑移速度、气固脉动能等更接近E-L方法模拟结果。颗粒聚团的积分尺度小于气相脉动速度的积分尺度,两者均呈各向异性,竖直分量高于水平分量。模拟得到了气固速度脉动关联系数和漂移速度系数。 展开更多
关键词 两相流 数值模拟 动力学理论 颗粒团聚 脉动关联项
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Effect of bed size on the gas-solid flow characterized by pressure fluctuations in bubbling fluidized beds 被引量:2
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作者 Jie Xiang yanguo zhang Qinghai Li 《Particuology》 SCIE EI CAS CSCD 2019年第6期1-9,共9页
Pressure fluctuations in four bubbling fluidized beds having different bed sizes (three square cross-sections of 5, 10, and 15 cm in side length, and one rectangular cross-section of 2 × 10 cm2) were measured at ... Pressure fluctuations in four bubbling fluidized beds having different bed sizes (three square cross-sections of 5, 10, and 15 cm in side length, and one rectangular cross-section of 2 × 10 cm2) were measured at four axial positions (P1, P2, P3, and P4). Several characteristic indicators of the flow specifically of the pressure were calculated. In terms of these characteristic indicators, the effect of bed size on flow behavior was investigated. The results show that in the fully fluidized state, the pressure drop is slightly higher in smaller beds, but the pressure drops in the 10- and 15-cm beds are close. The 15-cm bed has the lowest pressure-fluctuation amplitude. The amplitudes at P1 and P2 in the lower part of the bed are very close for bed sizes below 10 cm, but the amplitude at P3 near the bed surface increases with decreasing bed size. No general trend was observed regarding the effect of bed size on skewness and kurtosis of the pressure for all four axial heights. For the average, standard deviation, skewness, and kurtosis of the pressure at P4, the values are close for the two small beds (2 × 10 and 5 × 5 cm2) and the two large beds (10 × 10 and 15 × 15 cm2), and hence the effect of bed size separates the beds into two groups. In the fully fluidized state, for P1, P2, and P3, the Kolmogorov entropy and the dominant frequency both increase with increasing bed size, but in the pseudo-2D bed both are between the values for the 5- and 10-cm beds. 展开更多
关键词 Bubbling fluidized bed Pressure fluctuation Bed size Time-series analysis Dominant frequency Kolmogorov entropy
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Aerosol containment by airflow in biosafety laboratories 被引量:1
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作者 Xin Feng yanguo zhang +3 位作者 Zhonglin Xu Donglin Song Guoqing Cao Lei Liang 《Journal of Biosafety and Biosecurity》 2019年第1期63-67,共5页
In this paper,the progress and research related to aerosol containment by airflow in containment environments,e.g.,biosafety laboratories,are introduced from a mechanical engineering view.A good airdistribution strate... In this paper,the progress and research related to aerosol containment by airflow in containment environments,e.g.,biosafety laboratories,are introduced from a mechanical engineering view.A good airdistribution strategy in the room,a reasonable and stable pressure gradient in the containment area,and a necessary buffer room comprise the integral parts for regulating the air flow and providing the necessary containment.An optimal air-distribution strategy would reduce the residence time of the bioaerosol in the lab room and lower the exposure risk of the work staff.The pressure difference between adjacent rooms provides sufficient isolation protection when the door is closed.Nevertheless,an unfavorable air exchange would occur when the door is open,owing to door movement,passing people,or a tiny temperature difference.A buffer room is therefore necessary to offset the negative impact and maintain the containment effect. 展开更多
关键词 AEROSOL CONTAINMENT BIOSAFETY
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