Mechanochemistry approach was utilized to solve the carbon deposition during alkane pyrolysis process. Pt/Ni single-atom alloy (SAA) was constructed on Ni balls surface as catalyst and grinding medium simultaneously, and physical collision of metallic balls generated mechanical energy to remove the deposited carbon and accelerate reaction rates. XANES spectra proved Pt/Ni SAA structure on the Ni ball surface, and its turnover frequency (TOF) was 1530 h under 1 atm and 450 °C without by-products. An extremely long lifetime of methane pyrolysis at least 350 h on stream has been obtained. This Pt/Ni SAA was also active for mechano-pyrolysis of ethane/propane, and DFT calculations confirmed that the improvement of catalytic efficiency originated from the d-band center up-shifting under mechanic stress on Pt/Ni SAA surface. This mechanical catalysis study provides an alternative route for clean hydrogen production and a strategy for deposited carbon removal under mechanical conditions.

中文翻译：

---

Pt/Ni单原子合金促进烷烃机械热解制氢


采用力化学方法解决烷烃热解过程中的积碳问题。在镍球表面构建Pt/Ni单原子合金（SAA）同时作为催化剂和研磨介质，金属球的物理碰撞产生机械能去除沉积的碳并加速反应速率。 XANES光谱证明Ni球表面具有Pt/Ni SAA结构，其周转频率(TOF)在1atm和450℃下为1530h，无副产物。甲烷热解的使用寿命极长，至少可运行 350 小时。该 Pt/Ni SAA 对乙烷/丙烷的机械热解也具有活性，DFT 计算证实催化效率的提高源于 Pt/Ni SAA 表面机械应力下 d 带中心上移。这项机械催化研究提供了清洁氢气生产的替代途径以及机械条件下沉积碳去除的策略。