UiO-66-NH_(2)负载铜催化剂的制备及其对醇的催化氧化

通过溶剂热法成功制备了一种基于金属有机骨架(MOF)的复合材料Cu-Cu_(2)O/UiO-66-NH_(2),采用傅里叶变换红外光谱(FTIR)、X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)对材料进行全面表征。在空气作氧化剂条件下,以苯甲醇氧化为苯甲醛作为模型反应,系统地考察了溶剂、温度、催化剂各组分用量等因素对催化效果的影响。研究结果表明,该复合催化剂在醇选择性氧化反应中表现出优异的催化性能,60℃下反应5 h便可将苯甲醇定量转化为苯甲醛,并对其他苄基醇、烯丙基醇和杂芳基醇等底物也展现出良好活性。此外,循环利用3次后,该催化剂活性几乎不变,表明其具有良好的稳定性和重复使用性。

Synergetic enhancement of selectivity for electroreduction of CO_(2)to C_(2)H_(4)by crystal facet engineering and tandem catalysis over silver-incorporated-cuprous oxides

Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts.

Fe改性分子筛催化剂CH_(4)选择性催化还原N_(2)O

针对N_(2)O的CH_(4)选择性催化还原(CH_(4)-SCR),采用浸渍法制备了系列Fe改性分子筛(BEA、ZSM-5、SSZ-13)催化剂。实验结果表明:2%Fe-BEA(负载量2%(w))具有较高的催化活性,在进气(N_(2)O 40%(φ,下同),CH_(4)10%,N250%)总流量为50 mL/min、反应器气时空速为12000 h^(–1)的条件下,250℃时的N_(2)O转化率达99.5%,CH_(4)转化率达94.6%;反应器连续运行20 h,N_(2)O转化率基本保持不变,CH_(4)转化率仅略有下降。表征结果显示,2%Fe-BEA较高的催化活性与其易形成大量离子态Fe^(3+)活性物种密切相关,而2%Fe-SSZ-13更易形成大量FeOx物种,故在3种分子筛催化剂中催化活性最低。2%Fe-BEA上N_(2)O的CH_(4)-SCR遵循自由基反应机理,形成羟基自由基和甲氧基自由基,并可经进一步氧化,通过甲酸盐路径生成CO_(2)和H2O。

催化剂中Rh含量对NH_(3)及N_(2)O生成量影响研究

研究了不同Rh含量的三效催化剂对CO和NO_(x)的起燃性能,并对反应过程中副产物NH_(3)以及N_(2)O的生成规律进行研究。实验通过浸渍法制备得到不同Rh含量的Rh-Pd/Ce_(x)Zr_(1-x)O_(2)+La-Al_(2)O_(3)催化剂,采用一套专用多路固定床连续流动模拟气反应器对其性能进行评价。研究结果表明:不同Rh负载量表现出不同的N_(2)选择性,随着Rh用量的增加NO_(x)的转化性能提升。总体来看,低Rh用量的催化剂产生更多的N_(2)O和NH_(3)副产物,而随着Rh用量的增加其N_(2)选择性也增加。当温度达到400℃时,Rh用量≥0.141 g/L的催化剂基本没有N_(2)O生成,Rh用量≥0.283 g/L基本没有N_(2)O和NH_(3)生成。该研究对于优化三效催化剂中Rh配比以提升N_(2)选择性具有借鉴意义,并对于设计满足未来国Ⅶ排放标准的三效催化剂具有重要的指导意义。

Au/Cu_(2)O@Au可见光催化CO_(2)还原性能

为提高光催化还原二氧化碳(CO_(2))的产物产率和选择性,采用一步法在空腔氧化亚铜(Cu_(2)O)中引入金属Au,制备了Au/Cu_(2)O@Au光催化剂。通过XRD、SEM、TEM、XPS、紫外-可见吸收光谱等表征和光电化学性能测试对光催化剂进行分析,考察了Au/Cu_(2)O@Au光催化剂催化还原CO_(2)性能。结果表明:Au/Cu_(2)O@Au光催化剂具有优异的性能,在光照强度为20 mW/cm^(2)的可见光照射下,该光催化剂将CO_(2)光催化还原为甲烷(CH_(4))和一氧化碳(CO)的产率分别为4.86和42.04μmol/(g·h),选择性分别为31.62%和68.38%。与空腔Cu_(2)O光催化剂相比,CO产率提高了8.12倍,选择性提高了32.84百分点。一步法合成的Au/Cu_(2)O@Au光催化剂中的Au颗粒分布在Cu_(2)O的表面和空腔内部,独特的Au分布与空腔协同作用,提高了光催化剂对可见光的吸收能力、光生载流子分离能力和转移能力,有效抑制了光生载流子的复合,实现了CO产率和选择性的提高。

Low-Temperature Selective Catalytic Reduction of NO with NH_3 over Fe–Ce–O_x Catalysts

In this study,we used a simple impregnation method to prepare Fe-Ce-O_x catalysts and tested them regarding their low-temperature(200-300 ℃) selective catalytic reduction(SCR) of NO using NH_3.We investigated the effects of Fe/Ce molar ratio,the gas hourly space velocity(GHSV),the stability and SO_2/H_2O resistance of the catalysts.The results showed that the FeCe(1:6)O_x(Ce/Fe molar ratio is 1:6) catalyst,which has some ordered parallel channels,exhibited good SCR performance.The FeCe(1:6)O_x catalyst had the highest NO conversion with an activity of 94-99%at temperatures between 200 and300 ℃ at a space velocity of 28,800 h^(-1).The NO conversion for the FeCe(1:6)O_x catalyst also reached 80-98%between 200 and 300 ℃ at a space velocity of204,000h^(-1).In addition,the FeCe(1:6)O_x catalyst demonstrated good stability in a 10-h SCR reaction at200-300 ℃.Even in the presence of SO_2 and H_2O,the FeCe(1:6)O_x catalyst exhibited good SCR performance.

Study on methane selective catalytic reduction of NO on Pt/Ce_(0.67)Zr_(0.33)O_2 and its application

Monolithic catalysts of Pt/La-Al2O3 and Pt/Ce0.67Zr0.3302 were prepared to investigate methane selective catalytic reduction （SCR） of NO. The results indicate that Pt/Ce0.67Zr0.33O2 shows high activity and both NO and CH4 can be converted completely at 450℃. Meanwhile, NO and CH4 can be converted completely when there exists excess oxygen. The Pt/Ce0.67Zr0.33O2 catalyst were further investigated by using methane as reducing agent to SCR NO in a novel equipment which combined the CH4 selective catalytic reduction of NO with methane combustion. The result shows that the catalyst is high active and the novel equipment is very effective. The conversion of NO is above 92% under the conditions used in this work. The prepared burner and catalysts have great potential for application.

Selective and mild oxidation of sulfides to sulfoxides by H_2O_2 using DBUH-Br_3 as catalyst

DBUH-Br_3 catalyzed selective conversion of sulfides to sulfoxides in the presence of H_2O_2 as oxidizing agent is described.The reaction was performed selectively at room temperature and relatively short reaction times.

Morphology and Mechanical Properties of PS/Al_2O_3 Nanocomposites Based on Selective Laser Sintering

Selective laser sintering （SLS） is a new process to prepare the polystyrene （PS）/Al2O3 nanocomposites. In this paper, with different laser power and other processing parameters unchanged, the morphology, density and mechanical properties of the sintered specimens were investigated. It was found that nano-sized inorganic particles are uniformly located in the PS matrix and the maximum density of the sintered specimens with pure PS powder reaches 1.07 g/cm^3, higher than 1.04 g/cm^3 that of the sintered specimens with mixture powder. Due to strengthening and toughness of the nano-sized Al2O3 inorganic particles, the maximum notched impact strength and tensile strength of the sintered part mixed with nano-sized inorganic particles are improved greatly from 7.5 to 12.1 kJ/m^2 and from 6.5 to 31.2 MPa, respectively, under the same sintering condition.

Selective Oxidation of Toluene with Hydrogen Peroxide Catalyzed by V-Mo-based Catalyst

The selective catalytic oxidation of toluene with hydrogen peroxide over V-Mo-based catalysts under mild conditions was studied.The promotion effect of Mo on the catalysts was studied with V/Al2O3 and Mo/Al2O3 as reference samples.The catalysts were characterized by XRD,TPR,and XPS techniques.The results show that the addition of Mo to V/Al2O3 may change the distribution of V species on Al2O3 surface.Over V-Mo/Al2O3 catalyst,highly dispersed amorphous V species facilitates benzaldehyde formation,and crystalline V2O5 species increases the conversion of toluene but decreases the selectivity to benzaldehyde,while AlVMoO7 species favors both the conversion of toluene and the formation of cresols.The yield of benzaldehyde depends remarkably on the surface O/Al and Mo/V atomic ratios,and gets to a maximum value of 13.2% with a selectivity of 79.5% at an O/Al atomic ratio of 3.0 and Mo/V atomic ratio of 0.7.

Low-Temperature Denitrification Performance of Cu2O/Activated Carbon Catalysts for Selective Catalytic Reduction of NOx by CO

To improve the denitrification performance of carbon-based materials for sintering flue gas,we prepared a composite catalyst comprising coconut shell activated carbon(AC)modified by thermal oxidation air.The microstructure,the specific surface area,the pore volume,the crystal structure,and functional groups presented in the prepared Cu2O/AC catalysts were thoroughly characterized.By using scanning electron microscopy(SEM),nitrogen adsorption/desorption isotherms,Fourier-transform infrared(FTIR)spectroscopy and X-ray diffractometry(XRD),the effects of Cu2O loading and calcination temperature on Cu2O/AC catalysts were investigated at low temperature(150℃).The research shows that Cu on the Cu2O/AC catalyst is in the form of Cu2O with good crystalline performance and is spherical and uniformly dispersed on the AC surface.The loading of Cu2O increases the active sites and the specific surface area of the reaction gas contact,which is conducive to the rapid progress of the carbon monoxide selective catalytic reduction(CO-SCR)reaction.When the loading of Cu2O was 8%and the calcination temperature was 500℃,the removal rate of NOx facilitated by the Cu2O/AC catalyst reached 97.9%.These findings provide a theoretical basis for understanding the denitrification of sintering flue gas.

Effect of Cu Loading to Catalytic Selective CO Oxidation of CuO/CeO₂–Co₃O₄

This work studied CuO/CeO2-Co3O4 with wt% Ce:Co ratio 95:5 for selective CO oxidation with effect of? wt% Cu loading. The catalysts were prepared by co-precipitation. Characterizations of catalysts were carried out by XRD and BET techniques. The results showed a good dispersion of CuO for 5 wt% Cu loading catalysts and showed high specific surface area of catalyst. For selective CO oxidation, both 5CuO and 30CuO catalysts could remove completely CO in the presence of excess hydrogen at 423 K and 20CuO could eliminate CO completely at 443 K. Moreover, considering the selectivity to CO oxidation, the 5CuO catalyst has shown the highest selectivity of 85% while the 30CuO catalyst obtains the selectivity of 65% at the reaction temperature of 423 K.

Effect of pretreatment methods on the performance of Cu-Zr-Ce-O catalyst for CO selective oxidation

The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR and XPS techniques. The results showed that the Cu-Zr-Ce-O catalyst pretreated with oxygen exhibited the best catalytic performance and had the widest operating temperature window, with CO conversion above 99% from 160 to 200 ℃. The O2 pretreatment caused an enrichment of the oxygen storaged on the Cu active species and promoted the conversion of adsorbed oxygen into surface lattice oxygen. It also improved the amount of Cu＋/Cu^2＋ ionic pair, and then facilitated the formation of CuO active species on the catalyst for selective CO oxidation.

CYCLOSTATIONARITY-BASED OFDM SIGNAL SENSING OVER DOUBLY-SELECTIVE FADING CHANNELS

In this paper,using cyclostationarity-based sensing method to detect the presence of Orthogonal Frequency Division Multiplexing(OFDM) signal over doubly-selective fading channels is studied.By approximating the channel with Basis Expansion Model(BEM),we derive the second-order cyclostationary statistics of the received OFDM signal over doubly-selective fading channels.Theoretical analysis indicates that new cyclostationary signatures produced by Doppler spread and multipath delay can be further exploited in the detecting process.Simulation examples demonstrate that the sensing methods using channel-induced cyclostationary features provide substantial improvements on detection performance.

Selective Oxidation of Methane to Methanol Using Molecular Oxygen on MoOx/(LaCoO3+Co3O4)Catalysts

Comparatively high CH3OH selectivity (60.0%) and yield (6.7%) were obtained on MoOx/(LaCoO3+Co3O4) catalysts in selective oxidation of methane to methanol using molecular oxygen as oxidant. The interaction between MoOx and La-Co-oxide modified the molecular structure of molybdenum oxide and the ratio of O7O ' on the catalyst surface, which controlled the catalytic performance of MoOx/(LaCoO3+Co3O4) catalysts.

TRANSMIT ANTENNA SELECTION IN V-BLAST SYSTEM

In order to reduce the cost of Radio Frequency (RF) chains in the spatial multiplexing systems with Vertical-Bell Labs Layered Space-Time (V-BLAST) nonlinear receiver, a novel transmit antenna selection cri-terion is proposed with the motivation of minimizing the Vector Symbol Error Rate (VSER). In the proposed scheme, both the number of substreams and the mapping of substreams to antennas are dynamically adjusted based on the knowledge of channel. Simulation results illustrate that the proposed two-step selection criterion outperforms the existing eigenmode based selection criterion by 0.3dB at a VSER of 10?3.

Complexity-reduced ICI cancellation for OFDM system over doubly-selective channels

In doubly-selective fading wireless channel,the conventional orthogonal frequency division multi-plexing(OFDM)receivers for inter-carrier interference(ICI)compensation require extensive computa-tions.To obtain an effective balance between performance and complexity,the whole channel responsematrix was decomposed into a sequence of submatrix,and then a novel equalizer based on minimum meansquare error(MMSE)criterion was presented to combat the ICI.Furthermore,a simple ordering-baseddecision-feedback equalizer(DFE)was derived to exploit the temperal diversity gain offered by mobilechannels.Numerical studies illustrate that although the MMSE equalizer still suffers from error floor,whereas the DFE equalizer exhibits significant performance improvement.The advantage of the proposedscheme indicates its potential applications in the future broadband wireless systems.

Signal Detection for OFDM-IDMA Uplink over Doubly Selective Channels

Orthogonal frequency division multiplexing-interleave division multiple access (OFDM-IDMA) systems may suffer from serious inter-carrier interference (ICI) in time-and frequency-selective (doubly selective) channels. In such case, the conventional OFDM-IDMA detection algorithm for quasi-static channels will result in significantly performance degradation. In this paper, signal detection is investigated for OFDM-IDMA uplink over doubly selective channels. Firstly, the impact of time-varying channels for OFDM-IDMA uplink is analyzed, which leads to the failure of the conventional algorithm. Secondly, a novel iterative detection algorithm is developed based on an integrated interference canceller, which can iteratively estimate and mitigate the ICI as well as multiple access interference (MAI) simultaneously. In addition, an improved detection algorithm is derived for reducing the complexity using an approximation to the mean and variance of the interference. Simulation results indicate that the proposed algorithm can significantly enhance the system performance to the conventional case, and the improved algorithm can strike a balance between performance and complexity.

面向高速移动场景的OFDM系统信道估计综述

近年来,高速移动通信受到业界的广泛关注,其中接收机侧的信道估计直接决定了系统的通信质量。正交频分复用(orthogonal frequency division multiplexing,OFDM)以其高带宽效率和抗多径衰落的特性,在目前的无线通信中被广泛采用。综述了高速移动场景下OFDM系统信道估计方法;描述了OFDM的系统模型;分析了高速移动场景下信道的时间/频率选择性衰落特性(双选特性)和稀疏特性。基于深度学习和压缩感知的信道估计方法,其高精度和低复杂度被用于高速移动场景,该文分别对基于深度学习和压缩感知的信道估计算法进行了归纳、对比、分析,探讨了高速移动场景下信道估计的发展趋势。

光电探测设备的密封方法及O形圈密封设计

密封性作为光电设备的一项重要指标,会直接影响到光电设备的安全性、可靠性和耐久性。而O形圈是光电设备中一种重要且常见的密封形式。鉴于轴向密封的O形圈经常使用紧固螺栓进行压紧,该文章提出了一种基于国标的O形圈选型及沟槽和螺栓设计方法,并且对于其中的计算和查表部分基于Python进行了实现,在极大简化了设计流程、减少了设计计算量、提高设计效率的同时,对于标准件智能设计有一定的借鉴意义。