CO2预处理操作条件对Ni-Co双金属催化剂性能与结构的影响

与传统H₂预处理方法相比,新型H₂+CO₂预处理方法（HCD）能显著提升Ni-Co双金属催化剂的沼气重整活性及抗积碳性能. 考察了HCD预处理操作条件对催化剂性能与结构的影响. 较好的HCD预处理操作条件是在催化剂经H₂处理之后,再用175-200 mL·min^-1的原料气CH₄/CO₂（比例为0：10）在780-800 ℃下还原0.5-1h. 在优化预处理操作条件下对催化剂进行了511 h的耐久性考察,并运用X射线衍射（XRD）、热重-差示扫描量热（TG-DSC）、透射电子显微镜（TEM）等手段对耐久性测试后的催化剂进行了表征. 在511 h 的稳定性实验内,CH₄、CO₂转化率,H₂、CO选择性及H₂/CO体积比分别高达96%、97%,98%、99%及0.98. 催化剂在测试期间的平均积碳速率仅为0.2 mg·g^-1·h^-1. 在该预处理操作参数下,催化剂拥有最好的综合性能和良好的耐久性.     

泡沫镍载钌催化硼氢化钠水解制氢

应用化学镀法制备泡沫镍载钌(Ru)催化剂,以其用于燃料电池硼氢化钠(NaBH4)水解即时供氢.该催化剂具有稳定高效的活性和稳定性能,而泡沫镍的预处理是一重要步骤.研究了制氢过程中NaBH4浓度、反应温度及使用次数对产氢速率的影响.结果表明:产氢速率随温度的升高快速上升,当反应温度从15℃升高到60℃,产氢速率增加了十几倍;在NaBH4浓度为20%的3%NaOH溶液中,使用载Ru量为3%的催化剂,于23.5℃常压下,水解NaBH4,其产氢速率达到0.784 mL.s-1.g-1.这种容易制备的催化剂在多次使用后仍显示出较高的活性.     

热化学循环分解水制氢研究进展

热化学循环分解水制氢是利用核能或太阳能进行大规模、无污染制氢的有前景的方法 ,已经提出了多种流程.本文对热化学制氢流程及其评价标准进行了综述,重点介绍了碘硫循环、UT-3循环和Westinghouse循环等先进流程的研究进展.     

Ce掺杂K_2La_2Ti_3O_(10)催化剂的可见光高效催化制氢的研究

采用高温固相法合成了铈掺杂的K2La2Ti3O10催化剂,利用X射线衍射(XRD)、紫外-可见漫反射(UV-visDRS)、透射电镜(TEM)和X射线光电子能谱(XPS)对催化剂进行了表征.考察了催化剂的可见光催化分解甲醇水溶液制氢的活性,并对可见光催化机理进行了分析.研究表明,铈的掺杂没有改变K2La2Ti3O10的微晶结构,并使催化剂粒径有所减小.紫外可见漫反射分析表明禁带宽度为2.3eV左右,对可见光具有较高吸收.XPS表明La和Ti为+3和+4价,而Ce则是+3和+4的混合价态.担载2wt%Pt后,在可见光下光催化活性大大提高,当铈的掺杂量为0.5mol%(即Ce取代La的摩尔百分量)时,光催化活性达到最大,产氢速率为0.05mmol/h;光照5h后产氢量为0.22mmol,而纯K2La2Ti3O10的产氢量只有0.037mmol.     

微波辅助快速制备2D/1D ZnIn2S4/TiO2 S型异质结及其光催化制氢性能

The threat and global concern of energy crises have significantly increased over the last two decades. Because solar light and water are abundant on earth, photocatalytic hydrogen evolution through water splitting has been considered as a promising route to produce green energy. Therefore, semiconductor photocatalysts play a key role in transforming sunlight and water to hydrogen energy. To date, various photocatalysts have been studied. Among them, TiO₂ has been extensively investigated because of its non-toxicity, high chemical stability, controllable morphology, and high photocatalytic activity. In particular, 1D TiO₂ nanofibers (NFs) have attracted increasing attention as effective photocatalysts because of their unique 1D electron transfer pathway, high adsorption capacity, and high photoinduced electron–hole pair transfer capability. However, TiO₂ NFs are considered as an inefficient photocatalyst for the hydrogen evolution reaction (HER) because of their disadvantages such as a large band gap (~3.2 eV) and fast recombination of photoinduced electron–hole pairs. Therefore, the development of a high-performance TiO₂ NF photocatalyst is required for efficient solar light conversion. In recent years, several strategies have been explored to improve the photocatalytic activity of TiO₂ NFs, including coupling with narrow-bandgap semiconductors (such as ZnIn₂S₄). Recently, microwave (MW)-assisted synthesis has been considered as an important strategy for the preparation of photocatalyst semiconductors because of its low cost, environment-friendliness, simplicity, and high reaction rate. Herein, to overcome the above-mentioned limiting properties of TiO₂ NFs, we report a 2D/1D ZnIn₂S₄/TiO₂ S-scheme heterojunction synthesized through a microwave (MW)-assisted process. Herein, the 2D/1D ZnIn₂S₄/TiO₂ S-scheme heterojunction was constructed rapidly by using in situ 2D ZnIn₂S₄nanosheets decorated on 1D TiO₂ NFs. The loading of ZnIn₂S₄ nanoplates on the TiO₂ NFs could be easily controlled by adjusting the molar ratios of ZnIn₂S₄ precursors to TiO₂ NFs. The photocatalytic activity of the as-prepared samples for water splitting under simulated solar light irradiation was assessed. The experimental results showed that the photocatalytic performance of the ZnIn₂S₄/TiO₂ composites was significantly improved, and the obtained ZnIn₂S₄/TiO₂ composites showed increased optical absorption. Under optimal conditions, the highest HER rate of the ZT-0.5 (molar ratio of ZnIn₂S₄/TiO₂= 0.5) sample was 8774 μmol·g^-1·h^-1, which is considerably higher than those of pure TiO₂ NFs (3312 μmol·g^-1·h^-1) and ZnIn₂S₄nanoplates (3114 μmol·g^-1·h^-1) by factors of 2.7 and 2.8, respectively. Based on the experimental data and Mott-Schottky analysis, a possible mechanism for the formation of the S-scheme heterojunction between ZnIn₂S₄ and TiO₂ was proposed to interpret the enhanced HER activity of the ZnIn₂S₄/TiO₂heterojunctionphotocatalysts.      

纳米ZnO的制备及其在不同牺牲试剂下的光催化产氢性能

采用沉淀法与异相共沸蒸馏技术相结合制备了ZnO纳米粉体,并利用X射线粉末衍射、扫描电镜、透射电镜和液氮吸-脱附等技术对制备的样品进行了分析与表征．考察了Pt的负载量、煅烧温度以及牺牲试剂的种类和浓度对制备的纳米ZnO的光催化产氢效率的影响．结果表明：与其他温度下煅烧获得的产物相比,400 oC煅烧产物表现出最佳的光催化产氢效率,且以甲醇为牺牲试剂时纳米ZnO悬浮体系的光催化产氢效率远高于以三乙醇胺为牺牲试剂时的产氢效率．其原因在于光催化过程中甲醇氧化也对体系的产氢有贡献．此外,探讨了基于实验结果对含甲醇的     

甲醇水蒸气重整制氢Cu/ZnO/Al2O3催化剂的研究

燃料电池作为一种无污染、高效率的能源引起世界各大汽车公司的广泛关注[1,2]。用于燃料电池的燃料目前研究较多的是氢气,用氢气作燃料存在储存、安全、运输等问题,寻求合适贮氢方法或替代燃料,实现车载制氢是解决问题的办法。甲醇作为液体燃料,因具有高能量密度,低碳含量,以及运输和贮存等优势成为车载制氢的理想燃料,甲醇水蒸气重整制氢反应也成为研究的热点[3～10]。车载制氢对甲醇水蒸气重整制氢反应体系中的产氢速率,氢气和CO的含量都有一定的要求。尤其对CO含量要求更为苛刻,因CO易引起燃料电池阳极催化剂中毒[11,12]。因此,开…     

PbS插层K2Ti4O9催化剂：制备及光催化制氢活性

利用高温固相反应、离子交换、层间插入反应和硫化处理制备了PbS插层的K2Ti4O9催化剂。利用XRD、TEM、SEM、XRF、PL和紫外-可见漫反射光谱对催化剂进行了表征,考察了催化剂紫外光和可见光光催化制氢活性。结果表明,制备的PbS插层K2Ti4O9催化剂对可见光的吸收范围较宽,其吸收边界约为710 nm,在紫外光和可见光下3 h累积产氢量可达到115.46 mmol.gcat-1和0.92 mmol.gcat-1,与CdS插层K2Ti4O9催化剂相比具有更高的催化活性。     

钙钛矿型稀土复合氧化物催化剂上一氧化碳的选择氧化

考察了在钙钛矿型稀土复合氧化物催化剂上，氢气中一氧化碳选择氧化的催化性能，发现该催化剂具有优良的催化活性和选择性。LaMnO3中的锰被铜部分取代后可以提高其催化活性，当其中的镧再被锶或钡部分取代后所得的催化剂的催化活性进一步提高。其中以La0.8Sr0.2Mn0.5Cu0.5O3的催化活性为最佳，在该催化剂上，在40 000 mL·g－1·h－1下，155 ℃时CO可被完全转化为CO2，此时的选择性达54%，与铂催化剂的性能相近。反应气中加入CO2时，CO转化率下降，但选择性有所提高；加入水蒸气则使CO的转化率和反应选择性均下降。     

三元镍基硫属化物纳米棒阵列的简单合成及其高效的电催化析氧性能北大核心CSCD

通过一步溶剂热法成功合成了泡沫镍(NF)支撑的三元镍基硫属化物(Ni_(3)(Se_(x)S_(1−x))_(2))纳米棒阵列。结构表征结果表明,所得三元Ni_(3)(Se_(x)S_(1−x))_(2)纳米棒属于三方物相,在泡沫镍基底上形成了有序的阵列结构。由于其快速的载流子传输效率、丰富的活性位点和多阴离子的协同效应,Ni_(3)(Se_(0.3)S_(0.7))_(2)/NF纳米棒阵列具有最佳的电催化性能。在1.0 mol/L的KOH溶液中,电流密度为50 mA/cm2时,过电势仅为344 mV,塔菲尔斜率为40.17 mV/dec,同时具有优异的电化学稳定性。更重要的是,以商用Pt/C为阴极,Ni_(3)(Se_(0.3)S_(0.7))_(2)/NF纳米棒阵列为阳极进行全分解水实验,仅需要1.49 V的电池电位即可提供10 mA/cm2的电解电流,表现出良好的电解水效果。该研究为电解水技术领域提供了一种高效的电催化剂,也为电化学能源技术中非贵重电催化剂的合理构建提供了有价值的见解。