Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production
Achieving an exceptionally high loading of isolated cobalt single atoms on a porous carbon matrix for efficient visible-light-driven photocatalytic hydrogen production
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在多孔碳基质上实现极高的分离钴单原子负载量，以实现高效可见光驱动的光催化制氢
DOI：
10.1039/c8sc05540h
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发表时间：
2019-03-07
期刊：
影响因子：
8.4
通讯作者：
Dai, Sheng
中科院分区：
文献类型：
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作者：
Shi, Rui;Tian, Chengcheng;Dai, Sheng
单原子催化剂(SACs)在各种化学反应中显示出巨大的潜力，由于金属原子利用效率的最大化而成为催化领域最活跃的新前沿。制备SA的关键障碍在于开发合适的载体，以避免合成过程中的团聚或烧结。因此，实现隔离SA的高负载是不容易的，也是具有挑战性的。常规方法通常以极低的负载量(小于1.5wt%)形成SA。在这项工作中，开发了一种新的原位制备方法，该方法能够合成金属负载量高达5.9wt%的孤立钴(Co)SA。该方法基于富氮分子碳前体(1，4，5，8，9，12-六氮三苯基六碳腈)和CoCl2的简单一步热解。此外，由于成功地将电子从氮化碳转移到孤立的Co-SAS，我们证明了以Co-SAS为助催化剂的高效光催化制氢，其析出速率为1180mmolg(-1)h(-1)。我们预计，这项新的研究将激励发现更多具有高金属负载量的孤立的囊，明显推动这一新兴类型的先进催化剂的发展。
Single-atom catalysts (SACs) have shown great potential in a wide variety of chemical reactions and become the most active new frontier in catalysis due to the maximum efficiency of metal atom use. The key obstacle in preparing SAs lies in the development of appropriate supports that can avoid aggregation or sintering during synthetic procedures. As such, achieving high loadings of isolated SAs is nontrivial and challenging. Conventional methods usually afford the formation of SAs with extremely low loadings (less than 1.5 wt%). In this work, a new in situ preparation strategy that enables the synthesis of isolated cobalt (Co) SAs with an exceptionally high metal loading, up to 5.9 wt%, is developed. The approach is based on a simple one-step pyrolysis of a nitrogen-enriched molecular carbon precursor (1,4,5,8,9,12-hexaazatriphenylene hexacarbonitrile) and CoCl2. Furthermore, due to the successful electron transfer from carbon nitride to the isolated Co SAs, we demonstrate a high-performance photocatalytic H-2 production using Co SAs as a co-catalyst, and the evolution rate is measured to be 1180 mu mol g(-1) h(-1). We anticipate that this new study will inspire the discovery of more isolated SACs with high metal loadings, evidently advancing the development of this emerging type of advanced catalysts.