Hard carbon (HC) has emerged as a promising anode material for sodium-ion batteries (SIBs), however, it suffers from low specific capacity and inferior initial Coulombic efficiency (ICE). Herein, an oxygen-driven molecular reconfiguration strategy is proposed to strengthen reversible Na+ storage in HC through synergistic alkali activation and pre-oxidation. The oxygen functional groups on the surface promote the reconstruction of sp2-carbon within the highly cross-linked amorphous macromolecular coal precursor, thereby enabling the coal-based HC featuring with expanded interlayer spacing, increased pseudo-graphitic and closed-pore domains. This effectively facilitates the Na+ transport kinetics and stable Na+ (de)intercalation of HC, simultaneously suppressing the electrolyte decomposition. The resultant HC delivers a high reversible capacity of 317.4 mAh g-1 at 25 mA g-1, an impressive ICE of 88.05%, excellent rate capability of 253.42 mAh g-1 at 1000 mA g-1, and a superior capacity retention of 82.92% over 1000 cycles. This work highlights the crucial role of oxygen-driven microstructural reconstruction in durable sodium storage of HC.
This study utilized the cotton wool part of cigarette butts as a biomass precursor to synthesize ZnO@C-NA composite heterojunction (ZnO attached to a three-dimensional dendritic structure of carbon nanotubes) through a simple liquid phase deposition method. The composite structure of ZnO and C-NA has rich redox active sites and a large specific surface area. Compared with the three-dimensional dendritic carbon nanotube (C-NA) and ZnO anode (ZnO DS), the reversible capacity of the ZnO@C-NA anode is 627 mAh/g (200 cycles, 0.1 A) and 550 mAh/g (1000 cycles, 1 A). The synergistic effect of the carbon structure and zinc oxide component effectively improves the storage capacity of LIBs, accelerates the reaction kinetics, and effectively suppresses the volume expansion of zinc oxide during charging and discharging. This study provides a feasible strategy for developing novel negative electrode materials with rich resources and a simple synthesis route. The optimized heterojunction negative electrode has excellent Li+ storage performance and has good application prospects in advanced LIBs and other energy storage devices.
In this study, Ru catalysts supported on Ce-Al composite carriers were prepared using the precipitationhydrothermal method, significantly enhancing ammonia decomposition efficiency. The test results show that the Ru/3Ce-Al catalyst, with a Ru loading of only 0.8 wt%, achieves a reaction rate of 14.17 mmol gcat 500 degrees C, and reaches a 95 % conversion rate at 525 degrees C. No decline in efficiency was observed after 48 h of durability testing, which significantly reduces the usage of Ru. The RuO2 particle size in the samples was only 2-4 nm. Ce-Al composite increased the specific surface area and pore volume of the catalyst, facilitating the uniform distribution of Ru. Additionally, it increased the number of surface acidic sites and strengthened the metal-support interaction. The unique low redox potential and oxygen vacancies of CeO2 allowed for faster electron transfer to the Ru surface. DFT calculations revealed that bridge site adsorption was more stable, with the rate-determining step of the ammonia decomposition reaction being the formation of N2. Ce-Al composite catalysts enhanced NH3 adsorption strength and lowered the reaction energy barrier.
This study systematically investigates the mechanism of NOx emissions during the sintering process, with a focus on the utilization of biochar as an auxiliary fuel to replace a portion of the coke traditionally used in iron ore sintering. The research involved the simulation of sintering raw material ratios using iron ore, biochar, and coke powder. Substitution levels of biochar for coke were set at 0%, 20%, 40%, 50%, 60%, 80%, and 100%. NOx emissions during the sintering process were monitored using a sintering flue gas detection system. Simultaneously, a comprehensive analysis of the sintered ore was conducted with the aim of producing samples that meet sintered ore requirements while reducing. NOx emissions. Experimental results revealed that when biomass charcoal substitution for coke reached 50%, the lowest NO emissions were observed during the sintering process, with a reduction of over 90% in accumulated NO emissions in the exhaust gas. In this process, due to the participation of biochar, CO2 emissions were reduced by approximately 50% compared to traditional sintering processes. The study also analyzed the physicochemical properties of the sintered ore using methods such as XRD, Raman, FTIR, and Vickers hardness testing. The results indicated that the hardness fluctuated within the range of 610 to 710N for sintered products with different levels of biochar substitution, and there were minimal changes in Fe element content and crystal phase transformations.
This study introduces a combined heat and power (CHP) system primarily based on proton exchange membrane (PEM) fuel cells, which can provide electricity and heat for residential buildings in the East China region under two operating strategies. The analysis and discussion focus on the impact of parameters such as current density and gas inlet pressure on the system's output power and efficiency. The results indicate that excessively high current density decreases the system's electricity generation efficiency, while a moderate increase in hydrogen inlet pressure contributes to greater heat generation. Considering energy, economic, and environmental factors, the system operates with the thermal-led strategy in parallel with the grid, resulting in a substantial 73.3 % reduction in fuel costs. The annual greenhouse gas (GHG) emissions and the amount of emission reduction are lowered to 6.96 x 107 g and 3.39 x 107 g, respectively.
This study prepared a series of cerium oxide -based catalysts with different metal ruthenium loadings using an initial wet impregnation method. The results demonstrate that the prepared 1.4Ru/CeO2 catalyst exhibits outstanding catalytic performance and activity stability. Under the condition where the Ru loading is only 1.4 wt %, the catalyst achieves almost complete NH3 conversion at 500 degrees C, with a hydrogen production rate of 16.59 mmol gcat- 1 min -1. Furthermore, after a 48-h long-term test, the activity remains stable. Characterization tests show that the metal ruthenium is uniformly distributed on the surface of cerium dioxide, with particle sizes ranging from 3 to 6 nm. Notably, a structure characterized by lattice stripes overlapping between the metal and support is observed. Increasing the Ru loading can enhance the surface acidity sites of the catalyst and the interaction between the metal and the support, which plays a crucial role in the long-term stability of the catalyst. Additionally, the abundant oxygen vacancies in cerium dioxide and its low cerium oxidation-reduction potential facilitate electron transfer to ruthenium, enhancing the adsorption of NH3 and accelerating the desorption of N2.
Micromixers are essential components for controlling reactions in microfluidic devices, significantly enhancing their efficiency. This paper introduces an unbalanced separation and recombination micromixer with a circulating chamber and optimizes its geometric structure. The study investigates how the width ratio of the main subchannel and secondary subchannel, as well as the position of the circulating chamber, affect the mixing index and pressure drop at the micromixer's inlet and outlet. The enhanced mixing results from the unbalanced impact generated by the micromixer's separation and recombination, combined with the synergistic effect of fluid self-circulation. Simulation results indicate that the optimized micromixer achieves a mixing index close to 100 % when the Reynolds number exceeds 30, with a pressure drop of only 30 KPa at a Reynolds number of 50 in the micromixer's inlet and outlet. A microfluidic-based micromixer was fabricated using soft lithography and molding techniques. Liposomes were synthesized in a single step using soybean phospholipids, cholesterol, ethanol, and deionized water as raw materials. The micro-mixer exhibited exceptional mixing performance, enabling faster liposome synthesis compared to conventional methods. Additionally, the resulting liposomes exhibited smaller particle sizes and narrower size distributions. By adjusting the flow rates of the organic and water phases entering the micromixer, liposomes with a small particle size of 39 nm and a concentrated particle size distribution (PDI=0.104) were successfully produced. These findings highlight the microfluidic approach as a convenient, rapid, and efficient method for liposome preparation. Furthermore, the unbalanced separation and recombination micromixer with a circulating chamber demonstrated a simple structure, high mixing efficiency, and minimal pressure drop loss. It is versatile and suitable for various microreactor applications.
In this study, we prepared Mn-Co-Ce catalysts through coprecipitation, analyzed their physicochemical properties through X-ray diffraction, transmission electron microscopy, hydrogen temperature programmed reduction, and X-ray photoelectron spectroscopy, and studied the removal of NO by NH3+CO. The Ce-1.25 catalyst (Mn: Co: Ce molar ratio of 1:3:1.25) exhibited the highest NH3+CO synergistic NOx reduction efficiency. Doping of Ce at appropriate concentrations effectively mitigated the micro-agglomeration of metal particles, increasing the relative content of active species on the catalyst surface, providing more defect sites, and enhancing the electron mobility of the adsorbed species and catalyst. The mechanism of the CO-NH3-selective catalytic reduction (SCR) reaction synergy was revealed as follows. The CO-NO reaction involved the gradual deoxidization and reduction process of nitrate; it was difficult for this reaction to be activated in the later stages, which limited its overall activity. The NH3-SCR reaction on the sample surface followed the Langmuir-Hinshelwood mechanism, while CO oxidation and the CO-NO reaction mainly followed the Eley-Rideal mechanism. In the cooperative reaction process, CO mainly reacted with NO3* to generate NO2*, which was accompanied by direct oxidation of some CO.
烧结烟气中CO和NOx排放是当前大气污染治理的重点,但传统的NH3-SCR技术存在与烟气温度不匹配、CO处理方式不经济、氨逃逸严重等问题.为了探究CO协助NH3-SCR脱硝技术的规律,利用共沉淀法开发了一种以CoMnCe为活性成分的脱硝催化剂,可利用烧结烟气中的CO协同NH3脱除NOx,既可提高烟气中CO利用方式,又可降低NH3使用量.活性测试结果表明Ce物质的量比为0.75 时,其催化剂具有最佳协同脱硝效率,125℃下NO转化效率高达 98%;XRD、Raman、XPS、TEM、H2-TPR等表征结果表明催化剂中Ce物质的量比的增加抑制了Co3 O4中晶粒的生长,尽管Co3 O4和CeO2仍保持原有晶格结构,但仍有部分Co或Mn原子与Ce原子相互掺杂,导致金属晶格畸变,催化剂表面形成缺陷结构,并生成大量氧空位,同时Ce物质的量比较大时,导致CeO2覆盖催化剂表面结构,且过剩的CeO2在催化剂表面出现团聚现象,阻碍Mn和Co物种参与催化反应;催化活性测试发现制备的催化剂表现出一定抗氧抑制能力,特别是Ce物质的量比较低时,低温下CO-SCR反应活性较好,而随Ce物质的量比增加,催化剂抗氧抑制能力下降;同时随温度升高,表面氧在催化剂表面流动加快,从而促进反应进行,此时含Ce较多CMC2 催化剂表现出最佳的抗氧抑制性能,CO降低了NH3-SCR脱硝活性,但对于CMC0.75 催化剂,在相对较低温度下,其协同脱硝效率仍较高,这可能是由于催化剂含有的Co、Mn和Ce金属氧化物具有极高的氧化能力,因此合理控制不同金属间的比例与分布,可提高催化剂表面氧化能力,增强表面氧流动,增强协同催化活性.
Atomic layer deposition (ALD) is an efficient method to confine the Pt particles in the channels of KL zeolite to improve the durability of catalysts. However, the diffusion of metal precursors is impeded by the size of micropore. Herein, using polyethylene glycol (PEG) as zeolite growth modifier to limit the growth of KL zeolite in [001] direction, a unique KL zeolite with trimodal porosity (native and larger micropores, mesopores) was successfully synthesized. Hierarchically porous structure engineered the spatial location of Pt precursor during ALD process. The obtained micro/mesoporous structure favored the diffusion of the Pt precursor into the pores of KL zeolite, and led to the formation of highly dispersed Pt clusters in micropores, mesopores, and intersection of micro/mesopores of KL zeolite. The resultant Pt/KLP2 catalyst showed the enhanced n-heptane aromatization performances operated at low temperature (420 degrees C). Systematic characterizations reveal the synergetic effect of spatial environment of hierarchical porous KL zeolite promoted the n-heptane aromatization and molecular diffusion. Namely, micropores enhanced the n-heptane dehydrocyclization, and the mesopores with shortened diffusion length facilitated the mass transport of aromatics and inhibited secondary hydrogenolysis efficiently. The present work broadens the fundamental understanding of the role of zeolite channels for alkane reforming reactions.
以KMnO4、NaClO2为氧化剂进行模拟烟气吸收试验,探究单一碱液吸收剂、Na-K协同吸收剂对去除烟气中NOx的影响,引入微量SO2-3 离子对吸收效率进一步优化.结果发现,KOH碱液性能明显高于NaOH,30 min内KOH平均吸收率高达 99.4%,NaOH的平均吸收率仅 86.9%,这是K+离子半径更大,更易解离OH-所致.以 0.1 mol/L的KMnO4 作为氧化剂、双组份吸收液(n(Na)∶ n(K)= 1 ∶ 2,n为物质的量浓度)效率更高更稳定,30 min仍可达 86%,是双金属离子的电荷传递效应,使气相反应物向液相传递时气膜迅速破裂,减少了气液两相的扩散时间所导致,并通过DFT模拟计算充分证实了这一点.通过在吸收液中引入微量SO2-3 离子,平均吸收率提高了3%,证明SO2-3 离子进一步促进了硝酸盐物种的吸收转化.
A combined heat and power system (CHPs) using proton exchange membrane fuel cells (PEMFC) as its primary energy output device is an attractive option due to its high electrical generation efficiency and low heat-to-power ratio. A hybrid PEMFC-based CHPs (PEMFCCHPs) has been designed to provide both electricity and heat for a hydrogen high-speed service area. A comprehensive model of the system has been established and validated to analyze the impacts of key parameters such as PEMFC current density and anode hydrogen inlet pressure on the performance of hybrid PEMFC-CHPs. Evaluate and analyze the system from the perspectives of exergy, energy, and economy. The findings indicate that by fulfilling the service area's load demand, the thermal-led strategy can effectively prevent a waste of 670 kW of heat energy daily but exhibits a power shortage of 573.8 kW.& COPY; 2023 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
A series of CuMnOx catalysts were prepared the coprecipitation method to explore the effect of CO participation on NH3-SCR reaction. The result showed that the CM-3 sample reached 100% the conversion of CO and NO at a temperature lower than 175 ° C, this primarily occurs because the correct ratio of Cu and Mn is conducive to the formation of a solid solution, improves the synergy between Mn and Cu leads to stronger redox performance. Moreover, the interaction principle of CO participating in NH3-SCR reaction is thoroughly investigated through, in situ DRIFTS and DFT. First, NH3 has varying adsorption modes at different temperatures, at low temperatures, it predominantly combines with surface oxygen through hydrogen bonds; it is mainly a NH4+ species when it rises. Second, NH3 and CO compete for the same active center, which significantly affects the catalytic reaction on the sample surface. Further, it is confirmed that the deposition of CO32- is the main reason for the decline in of activity. Finally, the improvement in N2 selectivity in the reaction with CO participation is due to the N2O produced not being directly released, but being further reduced to N2 through species such as CO.
钢渣和污泥作为传统大宗固体废弃物,始终面临处理成本高、回收利用率低等问题,但其内部含有大量可利用物质,具有较高的资源化利用价值,现已成为国内外的研究热点.为了提高钢渣与污泥绿色、高效、协同资源化利用,综述了近年来国内外钢渣在建筑、道路、水处理、农业等领域资源化利用的研究进展,立足固废无害化、减量化,从钢渣和污泥的资源化进行分析与总结,指出不同研究方法的特点和优劣,为固废资源化利用提供参考.并基于我国发展现状对钢渣与污泥资源化利用的未来发展方向进行了展望,以期为固废处理行业的良性发展提供一定的理论支撑.
NO x and CO are the key pollutants to be treated. With the further improvement of flue gas emission standards such as steel sintering, the traditional NH 3 -SCR(NH 3 selective catalytic reduction of NO x ) denitration technology has significant shortcomings, especially the sintering flue gas emission temperature is lower than the window temperature of vanadium based catalysts, causing that the activity of vanadium based denitration catalyst is insufficient and the generated ammonium sulfide blocks the catalyst surface, but there is still a lack of effective means for CO control. Therefore, the development of low-temperature catalyst has become the key factor for removing NO x and CO from low-temperature flue gas. The progress of Mn based catalyst in removing NO x and CO was discussed, the effects of active components, preparation methods and supports on the catalytic activity of Mn based low-temperature catalyst were compared, and the effects of Cu、Ce and other metals on the modification of Mn based catalyst were introduced in detail, and the relationship between element doping and catalytic performance was analyzed. On this basis, the latest research results of no reduction technology by CO in recent years were systematically combed and summarized, and the reaction mechanism and the action mechanism of O 2 in the reaction were emphatically discussed. The results show that the rich extranuclear electron arrangement of Mn element is the fundamental reason for its excellent activity in removing NO x and CO, but most of the current research results are only in the laboratory theoretical stage and lack of large-scale verification in the actual flue gas. Finally, the future development direction of Mn based catalyst was prospected, and the catalyst deactivation mechanism and the scheme to improve the anti poisoning of catalyst were put forward.
In this study, Mn-Co bimetallic catalysts were prepared by a coprecipitation method. The effect of different Mn/Co molar ratios on the performance of NH3-SCR, CO-SCR, and CO oxidation was investigated, and a representative catalyst was selected to test the NOx catalytic activity of the NH3-CO-SCR synergy reaction. The microphysical and chemical properties of the samples were characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, and other analytical techniques. The CO-assisted NH3 removal mechanism of NOx was explored through in situ diffuse reflectance infrared spectroscopy (DRIFTS) and density functional theory (DFT). The results show that MC-3 has the best NOx catalytic activity and a wider SCR reaction temperature window. In the synergy reaction, the NOx conversion rate of NH3-SCR can be reached at NH3 = 400 ppm, and the N-2 selectivity is effectively improved. In situ DRIFTS and DFT results show that NH3-SCR follows the L-H mechanism. In the presence of CO, some CO competes with NH3 for adsorption on the Mn sites, which suppresses the adsorption activation of NH3 and reduces the CO oxidation activity. Second, with CO participation, the activation energy required for NH4NO3* to form is lower, which promotes its further decomposition into N-2 and H2O, and is of great significance for CO-assisted NH3 removal of NOx technology.
This study employed the water-thermal coupled high-temperature CO2 gasification method using Zhundong coal as the raw material to prepare porous carbon materials. A dual-function catalyst for NOx adsorption and reduction was prepared by loading Cu, Mn, and Ce components onto the carbon material through hydrothermal impregnation. The influence of metal loading content on the pore structure, surface functional groups, and synergistic effects between metals in the carbon-based catalyst was investigated during the preparation process. In the process of NOx removal using carbon-based catalysts, the primary components comprise two distinct phases: NOx adsorption and COSCR experiments. The experimental sequence involves the initial execution of NOx adsorption tests, succeeded by subsequent reduction treatments. These processes are undertaken systematically to comprehensively investigate the attributes of the catalyst. The physical and chemical parameters of the samples were characterized using XRD, Raman, H2-TPR, NOx-TPD, and other techniques. Finally, the NOx adsorption and reduction mechanism of representative samples were deeply analyzed using in situ DRIFTS. The results showed that when the loading amounts of Cu, Mn, and Ce were 0.006, 0.012, and 0.003 g, respectively, the pore structure of the catalyst was excellent, with a NOx adsorption performance (q(e)) of 16.23 mg/g, and the NO conversion rate reached 66% at 200 degrees C. This is mainly attributed to the enhanced interaction between metal species on the catalyst surface by optimizing the metal content on the carbon support, which promotes the dissociation of NO in the NO + CO reaction. In situ DRIFTS results confirmed that NO and CO adsorb on the catalyst surface, and CO* reacts with NO* to produce N-2 and CO2, following the Langmuir-Hinshelwood mechanism.
以木质素为原料,采用管式炉反应器通过一步热解-半活化法获得木质素基多孔炭材料(LPC).采用氮吸附(BET)、扫描电镜(SEM)和傅里叶变换红外光谱(FTIR)对多孔炭材料的物化性质进行分析.在900℃的恒定炭化温度下,CO2体积分数为6%、水蒸气体积分数约为20%时,LPC-C6S20表面具有良好的纳米结构,并且总孔容和比表面积分别达到0.77cm3/g和1497.51m2/g,活化气氛促进了多孔炭材料颗粒趋于均匀和微孔、中孔的形成.LPC样品含有—OH、C—H、C=C、C—O、C=O、CO—C、C—N、C=N等丰富的表面官能团.随着活化剂浓度的变化,这些官能团保持相对稳定.因此,通过该方法获得的样品具有良好的纳米结构,具有较大的孔容、比表面积和表面官能团.
芬顿铁泥是芬顿氧化技术处理工业有机废水产生的一种工业危险废弃物.芬顿铁泥中含有大量的铁资源,具有很高的资源回收潜力,现已成为国内外的研究热点.从化学法、热能法两个方面综述了目前国内外对芬顿铁泥的各类资源化利用方法,并对各类典型方法的研究进展、优缺点以及核心技术进行了介绍.展望了芬顿铁泥资源化利用未来的发展目标,并基于中国火电厂运行实际情况提出芬顿铁泥资源化利用新途径,即将芬顿铁泥作为原材料制备火电厂铁基选择性催化还原(SCR)脱硝催化剂,以期充分回收利用芬顿铁泥中的铁资源,减小铁泥堆积所造成的环境危害.
A series of coal-based materials were prepared using a hydrothermal method combined with high-temperature CO2 activation. During sample preparation, K modification was performed to optimize the surface functional groups and pore structure. The NOx adsorption volume of each sample was evaluated in a simulated flue gas atmosphere. The physical and chemical parameters of the samples were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, and temperature-programmed desorption of NOx and NO. In addition, the NOx adsorption mechanism of representative samples was explored by in situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculations. The adsorption capacity of NOx and SO2 with NOx was also systematically investigated using cyclic adsorption and co-adsorption experiments, respectively. The results showed that the optimized KOH concentration is 0.4 g KOH/30 mL H2O. At this concentration, the material had a relatively good pore structure and abundant surface functional groups. The investigation of the mechanism revealed that pore structure optimization is important for increasing the NOx adsorption capacity on the surface of the coal-based materials, followed by functional group and then surface metal optimization. In addition, oxygen-containing active functional groups with moderately high C-O and R2C=O contents can enhance the adsorption of NO to some extent. Optimizing the ratio of C-O to R2C=O is critical for NOx adsorption. This study is significant for NOx adsorption removal technology.