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991.
Juntian Niu Haiyu Liu Yan Jin Baoguo Fan Wenjie Qi Jingyu Ran 《Frontiers of Chemical Science and Engineering》2022,16(10):1485
Methane activation is a pivotal step in the application of natural gas converting into high-value added chemicals via methane steam/dry reforming reactions. Ni element was found to be the most widely used catalyst. In present work, methane activation on MgO supported Ni–M (M = Fe, Co, Cu, Pd, Pt) cluster was explored through detailed density functional theory calculations, compared to pure Ni cluster. CH4 adsorption on Cu promoted Ni cluster requires overcoming an energy of 0.07 eV, indicating that it is slightly endothermic and unfavored to occur, while the adsorption energies of other promoters M (M = Fe, Co, Pd and Pt) are all higher than that of pure Ni cluster. The role of M on the first C–H bond cleavage of CH4 was investigated. Doping elements of the same period in Ni cluster, such as Fe, Co and Cu, for C–H bond activation follows the trend of the decrease of metal atom radius. As a result, Ni–Fe shows the best ability for C–H bond cleavage. In addition, doping the elements of the same family, like Pd and Pt, for CH4 activation is according to the increase of metal atom radius. Consequently, C–H bond activation demands a lower energy barrier on Ni–Pt cluster. To illustrate the adsorptive dissociation behaviors of CH4 at different Ni–M clusters, the Mulliken atomic charge was analyzed. In general, the electron gain of CH4 binding at different Ni–M clusters follows the sequence of Ni–Cu (–0.02 e) < Ni (–0.04 e) < Ni–Pd (–0.08 e) < Ni–Pt (–0.09 e) < Ni–Co (–0.10 e) < Ni–Fe (–0.12 e), and the binding strength between catalysts and CH 4 raises with the CH4 electron gain increasing. This work provides insights into understanding the role of promoter metal M on thermal-catalytic activation of CH4 over Ni/MgO catalysts, and is useful to interpret the reaction at an atomic scale. 相似文献
992.
Wang Li Wen-Ying Li Xing-Bao Wang Jie Feng 《Frontiers of Chemical Science and Engineering》2022,16(12):1689
Radicals are important intermediates in direct coal liquefaction. Certain radicals can cause the cleavage of chemical bonds. At high temperatures, radical fragments can be produced by the splitting of large organic molecules, which can break strong chemical bonds through the induction pyrolysis of radicals. The reaction between the formation and annihilation of coal radical fragments and the effect of hydrogen-donor solvents on the radical fragments are discussed in lignite hydrogenolysis. Using the hydroxyl and ether bonds as indicators, the effects of different radicals on the cleavage of chemical bond were investigated employing density functional theory calculations and lignite hydrogenolysis experiments. Results showed that the adjustment of the coal radical fragments could be made by the addition of hydrogen-donor solvents. Results showed that the transition from coal radical fragment to H radical leads to the variation of product distribution. The synergistic mechanism of hydrogen supply and hydrogenolysis of hydrogen-donor solvent was proposed. 相似文献
993.
Siliu Lyu Muhammad Adnan Younis Zhibin Liu Libin Zeng Xianyun Peng Bin Yang Zhongjian Li Lecheng Lei Yang Hou 《Frontiers of Chemical Science and Engineering》2022,16(6):777
As an eco-friendly, efficient, and low-cost technique, photoelectrochemical water splitting has attracted growing interest in the production of clean and sustainable hydrogen by the conversion of abundant solar energy. In the photoelectrochemical system, the photoelectrode plays a vital role in absorbing the energy of sunlight to trigger the water splitting process and the overall efficiency depends largely on the integration and design of photoelectrochemical devices. In recent years, the optimization of photoelectrodes and photoelectrochemical devices to achieve highly efficient hydrogen production has been extensively investigated. In this paper, a concise review of recent advances in the modification of nanostructured photoelectrodes and the design of photoelectrochemical devices is presented. Meanwhile, the general principles of structural and morphological factors in altering the photoelectrochemical performance of photoelectrodes are discussed. Furthermore, the performance indicators and first principles to describe the behaviors of charge carriers are analyzed, which will be of profound guiding significance to increasing the overall efficiency of the photoelectrochemical water splitting system. Finally, current challenges and prospects for an in-depth understanding of reaction mechanisms using advanced characterization technologies and potential strategies for developing novel photoelectrodes and advanced photoelectrochemical water splitting devices are demonstrated. 相似文献
994.
Xiyuan Bu Ming Tian Hongqing Wang Lin Wang Liyong Yuan Weiqun Shi 《Frontiers of Chemical Science and Engineering》2022,16(11):1632
Although metal–organic frameworks offer a new platform for developing versatile sorption materials, yet coordinating the functionality, structure and component of these materials remains a great challenge. It depends on a comprehensive knowledge of a “real sorption mechanism”. Herein, a ternary mechanism for U(VI) uptake in metal–organic frameworks was reported. Analogous MIL-100s (Al, Fe, Cr) were prepared and studied for their ability to sequestrate U(VI) from aqueous solutions. As a result, MIL-100(Al) performed the best among the tested materials, and MIL-100(Cr) performed the worst. The nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(VI) uptake in the three metal–organic frameworks involves different mechanisms. Specifically, hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s (Al, Fe) by exchanging with hydrogen ions of terminal hydroxyl groups (Al-OH2, Fe-OH2), and/or, hydrated uranyl ions are bound directly to Al(III) center in MIL-100(Al) through a strong inner-sphere coordination. For MIL-100(Cr), however, the U(VI) uptake is attributed to electrostatic attraction. Besides, the sorption mechanism is also pH and ionic strength dependent. The present study suggests that changing metal center of metal–organic frameworks and sorption conditions alters sorption mechanism, which helps to construct effective metal–organic frameworks-based sorbents for water purification. 相似文献
995.
以玉米秸秆为原料, 利用热重分析法研究其热解的特性及动力学。根据TG和DTG曲线, 研究玉米秸秆的热解特性, 采用Flynn-Wall-Ozawa(FWO)和Kissinger-Akahira-Sunose(KAS)两种等转化率法计算玉米秸秆热解的活化能, 并结合主曲线法和Coats-Redfern(C-R)法探讨了玉米秸秆热解遵循的机理方程。研究结果表明: 玉米秸秆热解过程可分为干燥脱水、过渡、主热解和炭化4个阶段, 随着热解升温速率增大, TG和DTG曲线向高温侧偏移; 利用FWO和KAS法计算得到的表观活化能分别为181.7和181.5 kJ/mol; 利用主曲线法和C-R法求解出玉米秸秆热解的机理方程遵循Avrami-Erofeev方程, 当α=0.1~0.5时, n=3, f(α)=1/3(1-α)[-ln(1-α)]-2; 当α=0.5~0.7时, n=2, f(α)=1/2(1-α)[-ln(1-α)]-1。 相似文献
996.
工业基础类(industry foundation classes, IFC)文件是建筑信息模型的数据存储和交互的标准通用文件,其难以直接被用于数据分析和数据挖掘。图数据在描述数据间复杂关联关系时具有天然的优势,被大量应用于对关联关系的分析和挖掘中。建立从IFC文件到图数据库的自动映射机制,将IFC文件中的实体及其关联关系一一映射至图数据库的节点和关系中,并分析该自动映射机制的完备性和基于图数据库的信息管理效率。映射得到的基于图数据库的施工信息模型被应用于施工离散事件仿真、施工进度网络分析和施工延迟分析中。分析结果表明,提出的自动映射机制能够完整地传递基于IFC标准的信息,映射效率满足施工过程中信息高效交互的需求,且基于图数据的信息管理效率也高于直接操作IFC文件的效率。在此基础上,通过具体工程中施工进度信息的关系利用和挖掘体现所提数据映射机制的优越性,结果表明所提数据映射机制提高了预制装配式建筑施工管理效率。 相似文献
997.
【目的】乡野杂草是乡村生物多样性的重要组成部分,更是乡村生态系统的核心生物要素。长期以来,乡野杂草多样性的科学价值未得到足够重视,研究乡野杂草多样性特征及维持机制,并提出乡野杂草多样性保护策略,是乡村生物多样保护亟待解决的科学问题。【方法】选取四川东北丘陵区域典型传统村落蚕华山村为研究区域,对村落内乡野杂草种类及分布情况进行定性及定量调查。【结果】共记录乡野杂草65科188属263种,分布在院落、农田、水塘、沟渠、篱笆、崖壁、片林等21种不同类型的乡村生境中。分析发现,影响乡野杂草分布的主要环境因子为光照强度和土壤含水量,丰富多样的乡村生境类型为乡野杂草生长提供了多样化水热组合条件,而乡村生境多样性的维持与乡村生产生活方式密切相关。【结论】基于实证研究结果,在分析乡野杂草多样性维持机制的基础上,提出5项乡野杂草多样性保护策略:1)合理布局“三生”空间;2)修复重建“丘-田-林-塘-居”单元;3)保护乡村小微生境及构建立体生境网络;4)选用乡野杂草恢复乡村植被;5)传承传统乡村生态智慧。 相似文献
998.
999.
以赤泥、粉煤灰、脱硫石膏及一种碱性固体废弃物外加剂为胶凝材料,煤矸石为骨料,制备得到环境友好型全工业固废路面基层混合料(RFDC).研究了4个龄期(7、28、56、90 d)下,不同粉煤灰掺量RFDC无侧限抗压强度(fUCS)和劈裂抗拉强度(fSTS)的发展规律,分析了抗压试件和劈裂抗拉试件的破坏形态,探讨了固废胶凝材料中3种氧化物摩尔比与RFDC 7 d fUCS的相关性,揭示了RFDC的强度形成机理.结果表明:当粉煤灰掺量为15%时,RFDC的力学性能最佳,抗压试件为典型的中心抗压破坏,劈裂抗拉试件为煤矸石粗集料破坏;固废胶凝材料的n(CaO)/[n(SiO2)+n(Al2O3)]值与RFDC 7 d fUCS的相关性最高;钙矾石(AFt)、水化硅(铝)酸钙(C-(A)-S-H)凝胶及沸石类物质等水化产物是RFDC强度的主要来源. 相似文献
1000.
采用随机生成算法投放钢纤维,建立了随机乱向、定向钢纤维增强水泥基复合材料(SFRC、ASFRC)三点弯曲梁细观有限元数值模型,计算了不同纤维掺量下SFRC试件和ASFRC试件加载断裂的全过程,分析了三点弯曲梁开裂截面处的纤维应力,研究了定向钢纤维的细观增强机理.结果表明:SFRC试件和ASFRC试件荷载-裂缝张开口位移全曲线的模拟值与试验值符合较好,峰值荷载的误差在10%以内;SFRC试件和ASFRC试件的峰值荷载与纤维合力的最大值均随着纤维掺量的增加而增大,当纤维掺量为0.8%、1.2%、2.0%时,ASFRC试件的峰值荷载较SFRC试件提高了75%、111%、141%,纤维合力的最大值较SFRC试件增大了202%、144%、127%;定向钢纤维可以有效改善水泥基复合材料的断裂性能,显著提高钢纤维的利用率,延缓裂缝的扩展. 相似文献