Ruiqian Gu, Lixin Chen, Yingnan Zhao, Yue Ma, Tong‐Xing Wang, Rui‐Qi Yao, Tonghui Wang, Zi Yun Wen, Gao‐Feng Han, Xing‐You Lang, Q. Jiang
ABSTRACT Steam reforming of hydrocarbons is currently the dominant method for hydrogen (H 2 ) production. As a petroleum refining byproduct rich in butane and propane, liquefied petroleum gas (LPG) offers a more accessible and easily transportable alternative feedstock of hydrocarbons relative to methane‐enriched natural gas. However, conventional steam reforming of LPG requires high temperatures to cleave stable C─H bonds, and the inevitable release of carbon oxides as byproducts limits H 2 selectivity ( < 76 vol%). To overcome these limitations, we report a low‐temperature (37°C) mechanochemical strategy for converting LPG into high‐purity H 2 with chromium (Cr) powder. The reaction proceeds without carbon emissions and achieves a high H 2 selectivity of 97.2 vol%, far surpasses that of the thermochemical route (21.3 vol% at 800°C). The H 2 yield rate exhibits at least 50 times enhancement compared to thermochemistry. The H 2 yield ratio reaches 94.6%, nearly 13 times greater than thermochemistry (7.3%). Mechanistically, strong metal‐carbon interactions promote dehydrogenation and C─C bond cleavage, and metal‐hydrogen interactions determine H 2 selectivity. These findings highlight mechanochemistry as a promising low‐temperature, carbon‐free approach for sustainable H 2 generation.