Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

In this work, a series of Cu-ZSM-5 catalysts with different SiO₂/Al₂O₃ ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N₂, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N₂ selectivity was impacted by the Brønsted acidity and the isolated Cu²⁺ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.     

UV/H2O2 oxidation of tri(2-chloroethyl) phosphate: Intermediate products, degradation pathway and toxicity evaluation

Tri(2-chloroethyl) phosphate (TCEP) with the initial concentration of 5 mg/L was degraded by UV/H₂O₂ oxidation process. The removal rate of TCEP in the UV/H₂O₂ system was 89.1% with the production of Cl^? and PO₄^3? of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H₂O₂ system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^?1 (R²=0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO? and H₂O and the oxidation reaction with H₂O₂ were found during the degradation pathway of 5 mg/L TCEP in the UV/H₂O₂ system. For the first time, environment risk was estimated via the “ecological structure activity relationships” program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H₂O₂ system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.     

Advanced molecular-fingerprinting analysis of dissolved organic sulfur by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry using optimal spray solvent

Molecular level characterization of dissolved organic sulfur (DOS) by electrospray ionization-Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR MS) is necessary for further understanding of the role of DOS in the environment. Here, ESI spray solvent, a key parameter for ion production during ESI process, was investigated for its effect on the molecular characterization of DOS by ESI-FTICR MS. 100% MeOH as spray solvent was found for the first time to remarkably enhance the ionization efficiency of the majority of CHOS-molecules in NOM, which facilitated a total of 1473 CHOS-molecular formulas with one sulfur atom to be detected. The number of CHOS-molecular formulas obtained using 100%MeOH as spray solvent increased notably over 740 in comparison with those using 50% MeOH aqueous solution (731) or 50% ACN aqueous solution (653). Moreover, due to the enhancement of ionization efficiency of DOS during ESI processes, the tandem mass spectra of the NOM CHOS-molecules could be easily obtained using 100% MeOH as spray solvent, which were hardly obtained using 50% MeOH aqueous solution as spray solvent. The results of the tandem mass spectra suggested the first discovery of organosulfates or sulfonic acids in Suwannee River NOM sample. A simple method based on 100% MeOH as ESI spray solvent for advanced molecular characterization of DOS by ESI-FTICR MS was proposed and applied, and the results revealed more molecular information of DOS in sea DOM samples.     

Polycyclic aromatic hydrocarbons in benthos of the northern Bering Sea Shelf and Chukchi Sea Shelf

Eighteen polycyclic aromatic hydrocarbons (PAHs) were detected in benthos collected onboard the ‘Snow Dragon’ in the Northern Bering Sea Shelf and Chukchi Sea Shelf during the 6^th Chinese National Arctic Research Expedition (CHINARE 2014). Σ₁₈PAHs for all biota samples ranged from 34.2 to 128.1 ng/g dry weight (dw), with the highest concentration observed in fish muscle (Boreogadus saida) samples close to St. Lawrence Island. The PAH composition pattern was dominated by the presence of lighter 3 ring (57%) and 2 ring (28%) PAHs, indicating oil-related or petrogenic sources as important origins of PAH contamination. Concentrations of alkyl-PAHs (1-methylnaphthalene and 2-methylnaphthalene) were lower than their parent PAH (naphthalene) in all biological tissue, and their percentage also decreased significantly (p<0.05) compared with those in the corresponding sediment. There were no significant relationships between PAH concentrations and trophic levels, which is possibly due to the combined results of the complex benthic foodweb in the subarctic/Arctic shelf region, as well as a low assimilation/effective metabolism for PAHs. According to toxic potency evaluation results from TCDD toxic equivalents (TEQs) and BaP-equivalent (BaPE) values, whelk (Neptunea heros) and starfish (Ctenodiscus crispatus) are two macroinvertebrate species showing relatively higher dioxin-like toxicity and carcinogenic risk.     

轻质高强多功能点阵夹层结构研究进展

根据材料类型和点阵结构,对点阵夹层结构进行了分类简述,并从静态、动态力学性能上,分析了各类点阵夹层结构的优缺点。简要叙述了设计过程中,综合考虑材料、结构以及功能等影响因素,针对不同使用工况的要求,可对各影响因素进行匹配设计,以实现传热特性、电磁波屏蔽特性、声学特性等不同的功能性需求。然后介绍了复合点阵夹层结构(嵌锁组装、模具热压成形、穿插编织)和金属点阵夹层结构(冲压成形、挤压线切割、拉伸网折叠、搭接拼装、熔模铸造以及增材制造)的主要制造工艺。最后提出如何将设计因子与多目标进行匹配及优化设计,是轻质高强点阵夹层结构的重点研究方向,轻质高强点阵夹层结构将朝多材料及多结构复合方向发展,开发新的制造工艺,提高费效比,是点阵夹层结构材料需解决的问题。     

卤氧化铋光催化剂改性的研究进展及应用

随着全球环境问题与能源问题的不断加剧,人们迫切需要开发一些高效、环保、稳定的光催化剂。卤氧化铋(BiOX,X=Cl、Br、I)因其独特的层状结构,优异的光学、电学性能,在光催化领域受到了越来越多的关注。虽然BiOX光催化剂在光催化反应中展现出了优异性能,但其光催化效率仍有待提高。简要叙述了BiOX的结构与性能以及当前主流的制备方法,主要概述了最近几年卤氧化铋光催化剂改性的研究进展。改性方法主要有微结构调控、晶面与缺陷调控、掺杂、构造异质结等,这些方法主要是通过提高卤氧化铋或卤氧化铋复合物的光吸收能力、光生载流子的分离和运输效率、以及活性位点的暴露量来实现改性。介绍了其在环境、能源和生物等领域的应用,同时对BiOX的发展提出了问题和展望。     

资源科学的学科建设与人才培养模式的实践与思考

资源科学是自然科学、社会科学和工程技术科学相互交叉、相互渗透、相互结合的多学科横向发展的新学科领域,具有综合性、交叉性等学科特点。研究适应新时期面向国家和社会发展需求的资源科学学科建设与人才培养方向具有重要的科学与实践意义。在梳理资源科学的学科发展历程基础上,进一步探讨国内外高等院校资源科学的研究领域、学科体系建设、课程及专业设置和人才培养模式,总结了我国资源科学的学科建设和人才培养的成就与不足,以期更好地服务国家需求。     

三江源植被碳利用率动态变化及其对气候响应

本文基于MODIS GPP/NPP数据估算了三江源植被碳利用率（CUE）,结合气象数据和高程数据采用一元线性回归和相关分析法,探讨了2001~2017年三江源植被CUE的时空变化特征及植被CUE对气温、降水量和蒸散量变化的响应.结果表明：（1）三江源植被CUE年内3~10月表现为先增加后降低的变化趋势,其中6月植被CUE最高.（2）三江源年植被碳利用率位于0.73~1,平均水平为0.85;植被CUE空间上呈现北高南低,西高东低的分布特征.（3）整体上,三江源4~10月植被碳利用率与同期气温、降水量和蒸散量分别呈现正相关、负相关和负相关关系,降水量是影响三江源植被CUE变化的主要影响因素,气温为次要因素,蒸散量影响程度最小.     

烟花爆竹燃放对大气污染物及PM2.5组分影响

为了解烟花爆竹燃放对保定市大气污染物和PM_2.5中水溶性离子及有机碳（OC）、元素碳（EC）浓度的影响,对保定市春节期间大气污染物和颗粒物组分的浓度特征进行了分析,并评估了烟花爆竹的贡献.结果表明： 2019年春节期间烟花爆竹集中燃放期PM_2.5、PM₁₀、SO₂、NO₂、CO平均浓度比非集中燃放期分别增加了1.3、1.0、1.1、0.4、0.02倍;保定市春节期间禁燃措施施行后,除夕、初一2d污染物平均浓度、最高浓度和高浓度持续时间均明显下降,集中燃放期烟花爆竹燃放对PM_2.5、PM₁₀和SO₂浓度贡献量从50%左右（2018年、2017年）下降至30%左右（2019年）,其中SO₂贡献量下降幅度超过PM_2.5和PM₁₀;组分分析表明,接待中心站点（主城区）、涿州站点（区县建成区）烟花爆竹燃放期K⁺、Mg²⁺、Cl^-浓度在水溶性离子中的总占比分别为39.3%、51.1%,比非燃放期的占比显著上升;烟花爆竹燃放对PM_2.5中K⁺、Mg²⁺、Cl^-浓度贡献率在50%以上,其中对K⁺贡献占比高达89.0%,涿州站点SO₄^2-、K⁺、Mg²⁺、Cl^-的贡献量分别是接待中心站点的2.2、2.1、1.9、1.8倍,燃放期硫氧化率（SOR）、氮氧化率（NOR）相比于非燃放期均有一定程度的升高;集中燃放期OC、EC浓度较非集中燃放期分别升高了2.5、2.1倍,烟花爆竹燃放对OC影响大于EC.     

Well-to-wheels greenhouse gas and air pollutant emissions from battery electric vehicles in China

Mitigation and Adaptation Strategies for Global Change - Electric vehicles (EVs) play a crucial role in addressing climate change and urban air quality concerns. China has emerged as the global...