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用于增强甲烷光热干重整的三元肖特基-p-n异质结策略

Ternary Schottky-p-n heterojunction strategy for enhancing photothermal dry reforming of methane.

作者信息

Zhang Qingqing, Chen Ziyu, Ye Yutao, Xu Chang, Liu Cong, Cao Xiaoming, Zhang Jinlong, Lei Juying, Ye Ziwei, Wang Lingzhi

机构信息

State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Key Lab for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai 200237, China.

Shanghai Engineering Research Center for Multi-Media Environmental Catalysis and Resource Utilization, East China University of Science & Technology, Shanghai 200237, China.

出版信息

Sci Adv. 2025 Jul 18;11(29):eadv5078. doi: 10.1126/sciadv.adv5078.

Abstract

Breaking the trade-off between activity and stability in catalysts for dry reforming of methane has long remained a huge challenge. Here, we demonstrate a ternary Schottky-p-n (TSPN) heterojunction strategy based on Ni-NiO-SrNbO (NiO/SNO) for photothermal dry reforming of methane. This approach achieves a stable syngas production rate of 10.54 moles per gram per hour, with a light-to-fuel efficiency of 28.3% and a CH turnover frequency of 18 per second at 500°C generated by concentrated light irradiation. This low-temperature, high-rate activity benefits from the photoaccelerated CH-to-H process facilitated by the synergistic effect of NiO and Ni. Furthermore, the light-induced spatial separation of dual reduction sites for CO reduction (SNO) and H evolution (Ni) suppresses the reverse water-gas shift (RWGS) reaction, ensuring continuous supply of active oxygen and improving reaction stability. This finding is expected to substantially promote low-temperature photothermal catalytic technology in enhancing the selective conversion efficiency of C molecules.

摘要

长期以来,打破甲烷干重整催化剂活性与稳定性之间的权衡一直是一项巨大挑战。在此,我们展示了一种基于Ni-NiO-SrNbO(NiO/SNO)的三元肖特基-p-n(TSPN)异质结策略,用于甲烷的光热干重整。该方法实现了稳定的合成气产率为每克每小时10.54摩尔,在500°C下通过聚光照射产生的光-燃料效率为28.3%,CH转化频率为每秒18次。这种低温、高速率活性得益于NiO和Ni的协同效应促进的光加速CH到H的过程。此外,光诱导的用于CO还原(SNO)和H析出(Ni)的双还原位点的空间分离抑制了逆水煤气变换(RWGS)反应,确保了活性氧的持续供应并提高了反应稳定性。这一发现有望大幅推动低温光热催化技术提高C分子的选择性转化效率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3648/12273794/4c61eecf54b1/sciadv.adv5078-f1.jpg

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