Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2018-03-12 , DOI: 10.1016/j.apcata.2018.03.005 Andrei Veksha , Apostolos Giannis , Wen-Da Oh , Victor W.-C. Chang , Grzegorz Lisak , Teik-Thye Lim
Hydrogen chloride is commonly present in syngas produced from municipal solid waste and biomass gasification. The influence of HCl on the activity of nickel-based catalysts during catalytic naphthalene reforming was investigated. Two synthesized and two commercial catalysts were tested for steam reforming at 790 °C and SV 24,000 h−1. In the absence of HCl, nickel supported on limestone (Ni/Limestone) demonstrated lower naphthalene conversion (∼80%) compared to nickel supported on alumina (Ni/Alumina) and two commercial alumina supported catalysts (∼100%). In the presence of 2000 ppmv HCl, the naphthalene conversion of Ni/Limestone rapidly decreased due to the reaction with HCl and, probably, formation of molten CaCl2 deactivating the supported Ni nanoparticles. These data demonstrate limited applicability of calcium-based nickel catalysts for naphthalene reforming at the studied temperature. The efficiencies of Ni/Alumina and two commercial catalysts were maintained at ∼100% naphthalene conversion. However, HCl concentrations of 500–2000 ppmv had detrimental effect on water-gas shift activity of alumina supported catalysts during naphthalene reforming. The spent alumina supported catalysts were characterized by N2 adsorption, FESEM/EDS, XRD, XPS, TPR and TEM after the reforming in the absence and presence of HCl, and the results suggested that HCl increased nickel sintering in the catalysts causing the loss of water-gas shift activity. The losses of catalytic activity varied among the catalysts and were the lowest for Ni/Alumina, which contained nanosized porous alumina support and had the strongest Ni nanoparticle-support interactions.
中文翻译:
萘蒸汽重整过程中镍基催化剂的催化活性和对HCl中毒的抵抗力
从城市固体废物和生物质气化产生的合成气中通常存在氯化氢。研究了盐酸对催化萘重整过程中镍基催化剂活性的影响。测试了两种合成催化剂和两种商用催化剂在790°C和SV 24,000 h -1下的蒸汽重整。在没有盐酸的情况下,与负载在氧化铝上的镍(Ni /氧化铝)和两种市售氧化铝负载的催化剂(〜100%)相比,负载在石灰石上的镍(Ni /石灰石)表现出较低的萘转化率(〜80%)。在2000 ppmv HCl的存在下,Ni /石灰石的萘转化率由于与HCl的反应而迅速下降,并可能形成熔融的CaCl 2。使负载的Ni纳米颗粒失活。这些数据证明在所研究的温度下钙基镍催化剂在萘重整中的适用性有限。Ni /氧化铝和两种市售催化剂的效率保持在〜100%萘转化率。但是,在萘重整过程中,浓度为500-2000 ppmv的HCl对氧化铝负载的催化剂的水煤气变换活性有不利影响。用过的氧化铝负载的催化剂的特征在于N 2。重整后在不存在和存在HCl的条件下吸附,FESEM / EDS,XRD,XPS,TPR和TEM,结果表明HCl增加了催化剂中镍的烧结,从而导致水煤气变换活性的损失。催化剂活性的损失因催化剂而异,对于Ni /氧化铝而言是最低的,Ni /氧化铝含有纳米级多孔氧化铝载体,并且具有最强的Ni纳米颗粒-载体相互作用。