A semi-continuous process for co-production of CO2-free hydrogen and carbon nanotubes via methane pyrolysis

作者：Eddie Sun, Shang Zhai, Dohyung Kim, Marco Gigantino, Vasudev Haribal, Oliver S. Dewey, Steven M. Williams, Gang Wan, Alexander Nelson, Sebastian Marin-Quiros, Joel Martis, Chengshuang Zhou, Jinwon Oh, Richard Randall, Max Kessler, Dongjae Kong, Jimmy Rojas, Andrew Tong, Xintong Xu, Cassandra Huff, Matteo Pasquali, Raghubir Gupta, Matteo Cargnello, Arun Majumdar · 发表于：Cell Reports Physical Science · 年份：2023 · DOI：10.1016/j.xcrp.2023.101338 · 被引用次数：51 · 研究领域：Carbon Nanotubes in Composites、Catalysts for Methane Reforming、Hydrogen Storage and Materials

Heterogeneous catalytic pyrolysis of hydrocarbons to produce CO 2 -free hydrogen and high-quality solid carbon have historically been stymied by issues related to catalyst deactivation by carbon formed during pyrolysis on the catalyst surface. In addition, a system that demonstrates sustained performance in terms of high conversion, high H 2 yield, and high quality of produced carbon has remained elusive. Here, we propose and demonstrate a semi-continuous methane pyrolysis process to H 2 and carbon nanotubes (CNTs) consisting of repeated pyrolysis and in situ (i.e., within the reactor) CNT dislodging by vigorous steam/argon fluidization. With this process, we demonstrate 10 process cycles with high H 2 yield from CH 4 and CNT dislodging in a fluidized-bed reactor with an Fe/q-Al 2 O 3 catalyst synthesized by an easily scalable incipient wetness impregnation process. We also identify and present opportunities for future catalyst and process development.