Li Weisong, Song Yang, Nie Rongrong, Ni Lijun, Wu Di, Chu Ruizhi, Meng Xianliang
School of Chemical Engineering and Technology, China University of Mining and Technology, Xuzhou 221116, China.
School of Nuclear Equipment and Nuclear Engineering, Yantai University, Yantai 264005, China.
ACS Omega. 2025 Jul 28;10(30):33124-33137. doi: 10.1021/acsomega.5c02772. eCollection 2025 Aug 5.
To tackle the storage challenges for distributed hydrogen applications, the microwave-initiated methanol steam reforming (MSR) process was deployed to increase the flexibility and energy efficiency of the MSR hydrogen production. As the key, a series of carbon-supported CuZn catalysts were systematically investigated to reveal the impacts of dielectric properties, conductivity, and dispersion on the catalytic performance under microwave irradiation. In addition to the excellent dielectric properties and conductivity exhibited by the carbon supports, the efficient dispersion of active species will dominate the catalytic activity, which was evidenced by the fact that the graphite supported CuZnG-40 is less active than the carbon nanotube supported and well dispersed CuZnCNTs-10, even with CuZnG-40 presenting superior conductivity and dielectric properties. The high specific surface area, tubular structure, and abundant pores of the carbon nanotubes could significantly promote the dispersion of the CuZn active species, forming highly dispersed small CuO particles. The H-TPR indicated that the reduction temperature of the carbon nanotube supported CuZn can be as low as 175 °C and it is easy to generate highly active Cu/Cu sites. With a 1:1 (molar ratio) CHOH/HO feed and a weight hourly space velocity (WHSV) of 3 h, the microwave-initiated methanol conversion of the CuZnCNTs-40 reached 90% with a relatively low CO content at 250 °C.
为应对分布式氢应用中的存储挑战,采用了微波引发的甲醇蒸汽重整(MSR)工艺来提高MSR制氢的灵活性和能源效率。作为关键,系统研究了一系列碳载CuZn催化剂,以揭示介电性能、电导率和分散性对微波辐射下催化性能的影响。除了碳载体表现出的优异介电性能和电导率外,活性物种的有效分散将主导催化活性,这一点由以下事实证明:即使CuZnG - 40具有优异的电导率和介电性能,石墨负载的CuZnG - 40的活性仍低于碳纳米管负载且分散良好的CuZnCNTs - 10。碳纳米管的高比表面积、管状结构和丰富的孔隙可显著促进CuZn活性物种的分散,形成高度分散的小CuO颗粒。H - TPR表明,碳纳米管负载的CuZn的还原温度可低至175℃,且易于生成高活性的Cu/Cu位点。在CHOH/HO进料摩尔比为1:1和重量时空速(WHSV)为3 h⁻¹的条件下,CuZnCNTs - 40在250℃下的微波引发甲醇转化率达到90%,CO含量相对较低。