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Studies on QSAR of metalloporphyrin catalysts in the oxidation of cyclohexane to adipic acid

CHEN Yixia, SHE Yuanbin, XU Jing, LI Yan

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 155-161 doi: 10.1007/s11705-007-0029-1

摘要： The catalysis of chloridized metalloporphyrins in the oxidation of cyclohexane to adipic acid was systematically investigated. The turnover numbers (TON) data of 19 catalysts were obtained experimentally under optimal reaction conditions, and 2.4?10 TON for T(-Cl)PP-MnCl catalyst at 2.0?10 mol/L of dosage was reached under the conditions of dioxygen pressure of 2.5 MPa at 150?C for 4 h. This was the best result reported for this reaction up to now. The QSAR models for each concerned metalloporphyrin were established, where the catalytic activity was significantly correlated with the (the energy level of the lowest unoccupied molecule orbit) and L (the bond length between metal-nitrogen atoms). Using the QSAR models, four new metalloporphyrins with substituted nitro group were designed, and their catalytic activities were predicted. The experimental TON data of newly designed porphyrins were in good agreement with the predicted ones, and the square of their correlation coefficient was more than 0.958. The above results demonstrated that the proposed structure-activity relationship model could be applied to design some new metalloporphyrin catalysts, and to predict their catalytic activity in cyclohexane oxidation.

关键词： cyclohexane     concerned metalloporphyrin     structure-activity relationship     metal-nitrogen     oxidation    

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EFFECT OF EXOGENOUS ADDITIVES ON HEAVY METAL PASSIVATION AND NITROGEN RETENTION IN PIG MANURE COMPOSTING

《农业科学与工程前沿（英文）》 doi: 10.15302/J-FASE-2023487

摘要：

● Research on heavy metal passivation and nitrogen emissions is necessary for the pig industry.

关键词： additives     composting     heavy metals passivation     nitrogen retention     pig manure    

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Boron and nitrogen co-doped porous carbon derived from sodium alginate enhanced capacitive deionization

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2014-2024 doi: 10.1007/s11705-023-2346-4

摘要： Capacitive deionization can alleviate water shortage and water environmental pollution, but performances are greatly determined by the electrochemical and desalination properties of its electrode materials. In this work, B and N co-doped porous carbon with micro-mesoporous structures is derived from sodium alginate by a carbonization, activation, and hydrothermal doping process, which exhibits large specific surface area (2587 m2·g‒1) and high specific capacitance (190.7 F·g‒1) for adsorption of salt ions and heavy metal ions. Furthermore, the materials provide a desalination capacity of 26.9 mg·g−1 at 1.2 V in 500 mg·L‒1 NaCl solution as well as a high removal capacity (239.6 mg·g‒1) and adsorption rate (7.99 mg·g‒1·min‒1) for Pb2+ with an excellent cycle stability. This work can pave the way to design low-cost porous carbon with high-performances for removal of salt ions and heavy metal ions.

关键词： capacitance deionization     porous carbon     B/N co-doping     heavy metal ions     water purification    

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Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1782-1792 doi: 10.1007/s11705-022-2220-9

摘要： Ultra-dispersed Ni nanoparticles (7.5 nm) on nitrogen-doped carbon nanoneedles (Ni@NCNs) were prepared by simple pyrolysis of Ni-based metal–organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding anilines. Two different crystallization methods (stirring and static) were compared and the optimal pyrolysis temperature was explored. Ni@NCNs were systematically characterized by wide analytical techniques. In the hydrogenation of p-chloronitrobenzene, Ni@NCNs-600 (pyrolyzed at 600 °C) exhibited extraordinarily high performance with 77.9 h–1 catalytic productivity and > 99% p-chloroaniline selectivity at full p-chloronitrobenzene conversion under mild conditions (90 °C, 1.5 MPa H2), showing obvious superiority compared with reported Ni-based catalysts. Notably, the reaction smoothly proceeded at room temperature with full conversion and > 99% selectivity. Moreover, Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups (halogen, nitrile, keto, carboxylic, etc.), and could be easily recycled by magnetic separation and reused for 5 times without deactivation. The adsorption tests showed that the preferential adsorption of –NO2 on the catalyst can restrain the dehalogenation of p-chloronitrobenzene, thus achieving high p-chloroaniline selectivity. While the high activity can be attributed to high Ni dispersion, special morphology, and rich pore structure of the catalyst.

关键词： halogenated nitrobenzenes     room-temperature hydrogenation     Ni nanoparticles     nitrogen-doped carbon nanoneedles     metal–organic-framework    

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Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1114-1124 doi: 10.1007/s11705-021-2087-1

摘要： Improvement of the low-cost transition metal electrocatalyst used in sluggish oxygen evolution reaction is a significant but challenging problem. In this study, ultrafine Fe-modulated Ni nanoparticles embedded in a porous Ni-doped carbon matrix were produced by the pyrolysis of zirconium metal-organic-frameworks, in which 2,2′-bipyridine-5,5′-dicarboxylate operating as a ligand can coordinate with Ni2+ and Fe3+. This strategy allows formation of Fe-modulated Ni nanoparticles with a uniform dimension of about 2 nm which can be ascribed to the spatial blocking effect of ZrO2. This unique catalyst displays an efficient oxygen evolution reaction electrocatalytic activity with a low overpotential of 372 mV at 10 mA·cm–2 and a small Tafel slope of 84.4 mV·dec–1 in alkaline media. More importantly, it shows superior durability and structural stability after 43 h in a chronoamperometry test. Meanwhile, it shows excellent cycling stability during 4000 cyclic voltammetry cycles. This research offers a new insight into the construction of uniform nanoscale transition metals and their alloys as highly efficient and durable electrocatalysts.

关键词： metal-organic framework     pyrolysis     ultrafine     Fe-modulated Ni nanoparticles     oxygen evolution reaction    

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SUSTAINABLE NITROGEN MANAGEMENT IN AUSTRALIAN AGROECOSYSTEMS: CHALLENGES AND OPPORTUNITIES

《农业科学与工程前沿（英文）》 2022年 第9卷 第3期   页码 366-372 doi: 10.15302/J-FASE-2022447

摘要：

● There is huge potential for improvement of nitrogen management in Australia.

关键词： Australian agroecosystems     reactive nitrogen     sustainable development    

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SUSTAINABLE NITROGEN MANAGEMENT FOR VEGETABLE PRODUCTION IN CHINA

《农业科学与工程前沿（英文）》 2022年 第9卷 第3期   页码 373-385 doi: 10.15302/J-FASE-2022455

摘要：

● Sustainable nitrogen management strategies for Chinese vegetable production are summarized.

关键词： enhanced-efficiency nitrogen fertilizer     integrated knowledge and products strategy     nitrogen rate     reactive nitrogen loss     vegetable     yield    

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EFFECTS OF SUBSTITUTION OF MINERAL NITROGEN WITH ORGANIC AMENDMENTS ON NITROGEN LOSS FROM SLOPING CROPLAND

《农业科学与工程前沿（英文）》 2022年 第9卷 第3期   页码 396-406 doi: 10.15302/J-FASE-2022456

摘要：

● Interflow acts as the dominant pathway for N loss loadings.

关键词： improved fertilization regime     interflow     nitrogen forms     nitrogen leaching     purple soil     sloping cropland    

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Nitrogen distribution in the products from the hydrothermal liquefaction of sp. and sp.

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 985-995 doi: 10.1007/s11705-021-2126-y

摘要： The high contents of nitrogen-containing organic compounds in biocrude obtained from hydrothermal liquefaction of microalgae are one of the most concerned issues on the applications and environment. In the project, Chlorella sp. and Spirulina sp. were selected as raw materials to investigate the influence of different reaction conditions (i.e., reaction temperature, residence time, solid loading rate) on the distribution of nitrogen in the oil phase and aqueous phase. Three main forms of nitrogen-containing organic compounds including nitrogen-heterocyclic compounds, amide, and amine were detected in biocrudes. The contents of nitrogen-heterocyclic compounds decreased with temperature while amide kept increasing. The effect of residence time on the components of nitrogen-containing organic compounds was similar with that of temperature. However, the influence of solid loading rate was insignificant. Moreover, it was also found that the differences of amino acids in the protein components in the two microalgae might affect the nitrogen distribution in products. For example, nitrogen in basic amino acids of Spirulina sp. preferred to go into the aqueous phase comparing with the nitrogen in neutral amino acids of Chlorella sp. In summary, a brief reaction map was proposed to describe the nitrogen pathway during microalgae hydrothermal liquefaction.

关键词： microalgae     hydrothermal liquefaction     biocrude     nitrogen distribution    

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SOIL NITROGEN CYCLING AND ENVIRONMENTAL IMPACTS IN THE SUBTROPICAL HILLY REGION OF CHINA: EVIDENCE FROM

《农业科学与工程前沿（英文）》 2022年 第9卷 第3期   页码 407-424 doi: 10.15302/J-FASE-2022448

摘要：

● Soil nitrogen fluxes and influencing factors were reviewed in the subtropical hilly regions.

关键词： nitrogen cycling     soil nitrogen     nitrogen deposition     greenhouse gases emission     non-point source pollution     nitrogen use efficiency    

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PROGRESS ON IMPROVING AGRICULTURAL NITROGEN USE EFFICIENCY: UK-CHINA VIRTUAL JOINT CENTERS ON NITROGEN

《农业科学与工程前沿（英文）》 2022年 第9卷 第3期   页码 475-489 doi: 10.15302/J-FASE-2022459

摘要：

● Virtual joint centers on N agronomy were established between UK and China.

关键词： CINAg     N-CIRCLE     nitrogen use efficiency     reactive nitrogen     sustainable production    

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IMPROVING NITROGEN SAFETY IN CHINA: NITROGEN FLOWS, POLLUTION AND CONTROL

《农业科学与工程前沿（英文）》 2022年 第9卷 第3期   页码 465-474 doi: 10.15302/J-FASE-2022454

摘要：

● It is necessary to address the N flows and their impacts on environment in China for sustainable N management.

关键词： barriers     future management     ammonia emissions     nitrogen input     water N pollution    

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超重力环境下非金属氮掺杂石墨烯泡沫催化还原反应性能研究 Article

王志勇, 赵志建, Jesse Baucom, 王丹, Liming Dai, 陈建峰

《工程（英文）》 2020年 第6卷 第6期   页码 680-687 doi: 10.1016/j.eng.2019.12.018

摘要：

本文以硝基苯还原和亚甲基蓝降解为模型反应体系，以非金属氮掺杂石墨烯泡沫（NGF）作为三维结构式催化材料，研究了超重力环境对催化反应性能的影响。在超重力旋转圆管反应器内6484 g (g = 9.81 m·s–2)的超重力环境下，非金属催化硝基苯还原的表观速率常数是传统搅拌反应器内的6 倍。通过计算流体力学理论模拟，揭示了超重力旋转管式反应器内超重力水平较高，湍流动能比传统反应器内有显著提高，液固相表面更新速度快，提高了催化反应效率。X射线光电子能谱和拉曼光谱测试表明该催化材料组成和结构在超重力环境下的反应过程中保持稳定。在另一个模型反应体系中，非金属氮掺杂石墨烯泡沫催化亚甲基蓝降解的速率也随着超重力水平的增加而增大。这些结果表明了超重力强化非金属碳基催化材料催化还原反应的潜力。

关键词： 超重力技术     过程强化     非金属催化     碳基纳米材料     催化还原    

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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

《能源前沿（英文）》 doi: 10.1007/s11708-023-0908-2

摘要： The Haber-Bosch process is the most widely used synthetic ammonia technology at present. Since its invention, it has provided an important guarantee for global food security. However, the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental pollution. Under the serious pressure of energy and environment, a green, clean, and sustainable ammonia synthesis route is urgently needed. Electrochemical synthesis of ammonia is a green and mild new method for preparing ammonia, which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar, wind, or water energy, without greenhouse gas and toxic gas emissions. Herein, the basic mechanism of the nitrogen reduction reaction (NRR) to ammonia and nitrate reduction reaction (NO3− RR) to ammonia were discussed. The representative approaches and major technologies, such as lithium mediated electrolysis and solid oxide electrolysis cell (SOEC) electrolysis for NRR, high activity catalyst and advanced electrochemical device fabrication for NO3 − RR and electrochemical ammonia synthesis were summarized. Based on the above discussion and analysis, the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis     nitrogen     nitrate     nitrogen reduction reaction (NRR) to ammonia     nitrate reduction reaction (NO–3 RR)    

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A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications

《化学科学与工程前沿（英文）》   页码 1632-1642 doi: 10.1007/s11705-022-2187-6

摘要： 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.

关键词： U(VI)     metal–organic frameworks     adsorption mechanism     metal node    

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标题 作者 时间 类型 操作

Studies on QSAR of metalloporphyrin catalysts in the oxidation of cyclohexane to adipic acid

CHEN Yixia, SHE Yuanbin, XU Jing, LI Yan

期刊论文

EFFECT OF EXOGENOUS ADDITIVES ON HEAVY METAL PASSIVATION AND NITROGEN RETENTION IN PIG MANURE COMPOSTING

期刊论文

Boron and nitrogen co-doped porous carbon derived from sodium alginate enhanced capacitive deionization

期刊论文

Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed

期刊论文

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

期刊论文

SUSTAINABLE NITROGEN MANAGEMENT IN AUSTRALIAN AGROECOSYSTEMS: CHALLENGES AND OPPORTUNITIES

期刊论文

SUSTAINABLE NITROGEN MANAGEMENT FOR VEGETABLE PRODUCTION IN CHINA

期刊论文

EFFECTS OF SUBSTITUTION OF MINERAL NITROGEN WITH ORGANIC AMENDMENTS ON NITROGEN LOSS FROM SLOPING CROPLAND

期刊论文

Nitrogen distribution in the products from the hydrothermal liquefaction of sp. and sp.

期刊论文

SOIL NITROGEN CYCLING AND ENVIRONMENTAL IMPACTS IN THE SUBTROPICAL HILLY REGION OF CHINA: EVIDENCE FROM

期刊论文

PROGRESS ON IMPROVING AGRICULTURAL NITROGEN USE EFFICIENCY: UK-CHINA VIRTUAL JOINT CENTERS ON NITROGEN

期刊论文

IMPROVING NITROGEN SAFETY IN CHINA: NITROGEN FLOWS, POLLUTION AND CONTROL

期刊论文

超重力环境下非金属氮掺杂石墨烯泡沫催化还原反应性能研究

王志勇, 赵志建, Jesse Baucom, 王丹, Liming Dai, 陈建峰

期刊论文

Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

期刊论文

A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications

期刊论文