Nature Communications ( IF 14.7 ) Pub Date : 2023-02-13 , DOI: 10.1038/s41467-023-36407-1
Kyungho Lee, Paulo C. D. Mendes, Hyungmin Jeon, Yizhen Song, Maxim Park Dickieson, Uzma Anjum, Luwei Chen, Tsung-Cheng Yang, Chia-Min Yang, Minkee Choi, Sergey M. Kozlov, Ning Yan
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Metal promotion is the most widely adopted strategy for enhancing the hydrogenation functionality of an oxide catalyst. Typically, metal nanoparticles or dopants are located directly on the catalyst surface to create interfacial synergy with active sites on the oxide, but the enhancement effect may be compromised by insufficient hydrogen delivery to these sites. Here, we introduce a strategy to promote a ZnZrOx methanol synthesis catalyst by incorporating hydrogen activation and delivery functions through optimized integration of ZnZrOx and Pd supported on carbon nanotube (Pd/CNT). The CNT in the Pd/CNT + ZnZrOx system delivers hydrogen activated on Pd to a broad area on the ZnZrOx surface, with an enhancement factor of 10 compared to the conventional Pd-promoted ZnZrOx catalyst, which only transfers hydrogen to Pd-adjacent sites. In CO2 hydrogenation to methanol, Pd/CNT + ZnZrOx exhibits drastically boosted activity—the highest among reported ZnZrOx-based catalysts—and excellent stability over 600 h on stream test, showing potential for practical implementation.
中文翻译:

设计纳米级 H 供应链以加速 ZnZrOx 上的甲醇合成
金属促进是最广泛采用的增强氧化物催化剂加氢功能的策略。通常,金属纳米粒子或掺杂剂直接位于催化剂表面,以与氧化物上的活性位点产生界面协同作用,但增强效果可能会因输送到这些位点的氢气不足而受到影响。在这里,我们介绍了一种策略,通过优化集成负载在碳纳米管 (Pd/CNT) 上的ZnZrO x和 Pd,结合氢活化和输送功能来促进 ZnZrO x甲醇合成催化剂。Pd/CNT + ZnZrO x系统中的 CNT将 Pd 上激活的氢传递到 ZnZrO x上的广阔区域表面,与传统的 Pd 促进的 ZnZrO x催化剂相比,增强因子为 10,后者仅将氢转移到 Pd 相邻位点。在 CO 2加氢制甲醇中,Pd/CNT + ZnZrO x表现出显着提高的活性(在已报道的 ZnZrO x基催化剂中最高)和超过 600 小时的运行测试的出色稳定性,显示出实际应用的潜力。