Promotional effect of ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and its synergic application with Fe/Beta catalysts

• K⁺ hinder the structural degradation of Cu/SAPO-34 under humid condition<100°C. • K⁺ on Cu/SAPO-34 brings lower acidity and inferior SCR activity at high temperature. • Fe/Beta was used to compensate the low activity of Cu/SAPO-34 at high temperature. • The hybrid catalysts with KCu/SAPO-34 and Fe/Beta show a great potential for using. K ions were introduced onto Cu/SAPO-34 catalysts via the ion-exchange process in order to improve their stability under low-temperature hydrothermal aging. The changes in structure and copper-species contents of these catalysts upon hydrothermal aging were probed in order to investigate their effects on selective catalytic reduction (SCR) activity. For the fresh Cu/SAPO-34 catalysts, K ions had little influence on the chabazite framework but effected their acidities by exchanging with acid sites. After hydrothermal aging, the structural integrity and amount of active sites decreased on pure Cu/SAPO-34. While the K-loaded catalysts showed improved chabazite structure, acidity, and active site conservation with increasing K loading. However, although the 0.7 wt% K catalyst maintained the same crystallinity, active site abundance, and low-temperature SCR activity as the fresh catalyst upon aging, an apparent decrease in SCR activity at high temperature was observed because of the inevitable decrease in the number of Brönsted acid sites. To compensate for the activity disadvantage of K-loaded Cu/SAPO-34 at high temperature, Fe/Beta catalysts were co-employed with K-loaded Cu/SAPO-34, and a wide active temperature window of SCR activity was obtained. Thus, our study reveals that a combined system comprising Fe/Beta and K-loaded Cu/SAPO-34 catalysts shows promise for the elimination of NO_x in real-world applications.     

褐煤脱水及水质净化研究

为实现褐煤提质并缓解褐煤产区缺水现状,采用微波及水热脱水方法对褐煤进行脱水改性并回收褐煤所脱水分.通过检测水分化学需氧量、氨氮、总磷、硬度、离子、有机化合物等各项指标,对褐煤中水分进行深入分析,并比较两种脱水方法的脱水、净化效果.结果表明微波方式脱水率可达70%~80%,除化学需氧量外,其它水质指标均符合工业用水标准,且杂质含量随微波功率增加而降低,利于净化回收.水热方式可有效改善褐煤煤质,脱水率最高可达87.44%,但各项水质指标均大大超出标准范围,且杂质含量在250℃工况下达到最大.两种冷凝水均检测到微量有毒金属元素、有毒致癌的多环芳烃及酚类化合物,将成为后续净化的主要脱除对象.     

TiO_2中空微球的制备及其对罗丹明B的光催化降解

采用一步水热法,以TiCl_4,H_2O_2,KBF4为原料,制备了TiO_2中空微球。采用SEM和XRD技术对TiO_2中空微球的形貌和结构进行了表征。以罗丹明B为模拟降解物,研究了TiO_2中空微球的光催化降解活性;并对TiO_2中空微球的生长机制进行了探讨。表征结果显示,制得的TiO_2中空微球呈锐钛矿型,颗粒分散均匀,外径约为3μm。实验结果表明,在紫外光照射下,加入1 g/L的TiO_2中空微球,处理初始质量浓度为20 mg/L、溶液p H为7的罗丹明B溶液,降解时间为120 min时,罗丹明B降解率可达93.38%。     

Zr\TiO2纳米管的制备及其光催化活性的初步研究

采用水热合成法以锐钛型Zr/TiO2纳米粒子为原料制备了掺杂锆二氧化钛纳米管,用TEM、EDS、BET对其进行了表征.结果表明,采用水热合成法制备的纳米管,其形貌均一,多层管壁.比表面积达到了291 m2·g-1,远远大于Zr/TiO2纳米颗粒的比表面积(76 m2·g-1).以罗丹明B为目标降解物的光催化实验表明,与Zr/TiO2纳米颗粒相比,Zr/TiO2纳米管的光催化活性有了显著的提高.     

Hydrothermal fabrication and visible-light-driven photocatalytic properties of bismuth vanadate with multiple morphologies and/or porous structures for Methyl Orange degradation

Monoclinic BiVO₄ with multiple morphologies and/or porous structures were fabricated using the hydrothermal strategy. The materials were characterized by means of the XRD, Raman, TGA/DSC, SEM, XPS, and UV-Vis techniques. The photocatalytic activities of the BiVO₄ materials were evaluated for the degradation of Methyl Orange under visible-light irradiation. It is observed that pH value and surfactant exerted a great effect on the morphology and pore structure of the BiVO₄ product. Spherical BiVO₄ with porous structures, flower-cluster-like BiVO₄, and flower-bundle-like BiVO₄ were generated hydrothermally at 100℃ with poly(vinyl pyrrolidone) (PVP) and urea (pH = 2) and at 160℃ with NaHCO₃ (pH = 7 and 8), respectively. The PVP-derived BiVO₄ showed much higher surface areas (5.0-8.4 m²/g) and narrower bandgap energies (2.45-2.49 eV). The best photocatalytic performance of the spherical BiVO₄ material with a surface area of 8.4 m²/g was associated with its higher surface area, narrower bandgap energy, higher surface oxygen vacancy density, and unique porous architecture.     

水热法制备纳米TiO_2处理垃圾渗滤液的实验研究

以钛酸四正丁酯为原料,采用水热法制备纳米TiO_2材料,经过高温煅烧后,对其降解垃圾渗滤液的催化活性进行测定,并用XRD,TEM和UV-Vis对其晶体结构进行表征。实验结果表明,水醇比、水热温度和酯加入量对TiO_2催化效率有显著的影响,当水醇比为1∶3、煅烧温度500℃、水热时间4 h、Ti(OC_4H_9)_4加入量为10 m L条件下制备的TiO_2粉末光催化活性最好,对垃圾渗滤液的降解在180 min时均可以达到73%,COD的去除率可达76.92%。     

废轮胎流化床热解半焦结构特性

以流化床反应器为主体对废轮胎热解半焦微观结构特性进行了研究.主要研究了热解温度、床料粒径、流化数等参数对热解半焦的比表面积、孔隙率、孔体积的影响.结果表明:半焦比表面积和孔隙率随温度变化过程中会在650℃或750℃出现一峰值,这表明对半焦品质而言,轮胎存在最佳的热解温度,采用较小粒径(0.135～0.304mm)床料时有使最佳热解温度下降的趋势;半焦孔隙率随流化数增加而减小;半焦比表面积随流化数的变化趋势与热解温度有关,550℃时流化数增加半焦比表面积减小,650℃时流化数增加半焦比表面积增大;半焦孔体积随温度的变化趋势与床料粒径有关,采用较大粒径(0.304～0.4mm)床料时,半焦孔体积随温度升高呈现先降后升的趋势,而采用较小粒径(0.135～0.304mm)床料时,半焦孔体积随温度升高呈现下降的趋势.     

不同酸碱条件下胶体迁移对含水介质渗透性的影响

文章通过室内土柱实验,研究胶体在迁移过程中对含水介质渗透性的影响以及不同酸碱条件下含水介质渗透性变化的特征,并从胶体的动电性质、粒径分布以及胶体与含水介质的空间排斥效应等方面对含水介质渗透性变化的微观机理进行探讨。研究结果表明,胶体溶液的酸碱度对含水介质的渗透性影响很大,中性和碱性条件下,胶体容易迁移,含水介质渗透性变化小。不同酸碱度条件下胶体粒度、表面动电性质不同:在酸性环境下出水胶体表面zeta电势和淌度为正,由于胶体带正电荷与含水介质表面所带负电荷的电性相反,电荷之间的吸引作用使胶体沉积作用加大,随着胶体聚沉在含水介质表面上渗透性急剧降低;在碱性环境中出水胶体表面zeta电势和淌度为负,电荷间的排斥作用将极大地促进胶体在含水介质中的迁移。     

水热炭化对吸附处理染料废水产生的废活性炭的再生效果

为实现废粉末活性炭的循环利用,采用水热炭化对吸附处理染料废水产生的废粉末活性炭进行再生,考察了水热炭化再生温度、再生时间、初始pH和再生次数等因素对废粉末活性炭再生效果的影响.结果表明:将320℃的水热条件下反应8 h得到的再生粉末活性炭用于吸附处理染料废水,色度去除率在95%左右,废粉末活性炭再生率可超过60%,且酸性条件下更有利于活性炭再生.经过5次吸附再生循环,废粉末活性炭再生率为55.54%,再生率仅下降6.06%.红外光谱分析结果表明,新粉末活性炭、废粉末活性炭和再生粉末活性炭的官能团种类基本一致;表面官能团Boehm滴定测定结果显示,再生粉末活性炭表面碱性基团含量降低、酸性基团含量增加.由于升温改变了废粉末活性炭的吸附平衡,有机物从其表面脱附,部分有机物在再生液中降解;此外,废粉末活性炭表面不易挥发和脱附的有机物在高温高压下炭化所得的产物能进一步吸附有机物,因此导致了废粉末活性炭的再生.研究显示,水热炭化对废粉末活性炭有较好的再生效果,具有实际应用价值.      

Bi_2MoO_6可见光催化去除4BS染料实验研究

以Bi(NO_3)_3·5H_2O和(NH_4)_6M_o7O_(24)·4H_20为原料,采用预超声-水热法合成可见光催化剂Bi_2MoO_6,考察了在可见光催化条件下,催化剂的用量、污染物初始浓度、溶液pH值等因素对偶氮染料直接耐酸大红4BS去除效果的影响.结果表明,4Bs溶液初始浓度为20mg·l~(-1)、原始pH值6.90条件下,催化剂的最佳投加量为2g·l~(-1),光照60min后,4BS去除率达到92.7%;在实验浓度20-100mg·l~(-1)的范围内,催化剂投加量为2.0g·l~(-1),光照210min后染料去除量最大可达到约50mg·l~(-1),溶液在弱酸或弱碱性条件下脱色较为稳定,在强酸或强碱性条件下脱色较快,效果明显;催化剂重复使用前后结构和成分稳定,但光催化活性有所下降.