Nature Communications ( IF 14.7 ) Pub Date : 2019-08-19 , DOI: 10.1038/s41467-019-11796-4 Zhengkun Yang 1 , Bingxu Chen 2 , Wenxing Chen 3 , Yunteng Qu 1 , Fangyao Zhou 1 , Changming Zhao 1 , Qian Xu 4 , Qinghua Zhang 5 , Xuezhi Duan 2 , Yuen Wu 1, 6
Single-atom metal catalysts have sparked tremendous attention, but direct transformation of cheap and easily obtainable bulk metal oxide into single atoms is still a great challenge. Here we report a facile and versatile gas-transport strategy to synthesize isolated single-atom copper sites (Cu ISAS/NC) catalyst at gram levels. Commercial copper (I) oxide powder is sublimated as mobile vapor at nearly melting temperature (1500 K) and subsequently can be trapped and reduced by the defect-rich nitrogen-doped carbon (NC), forming the isolated copper sites catalyst. Strikingly, this thermally stable Cu ISAS/NC, which is obtained above 1270 K, delivers excellent oxygen reduction performance possessing a recorded half-wave potential of 0.92 V vs RHE among other Cu-based electrocatalysts. By varying metal oxide precursors, we demonstrate the universal synthesis of different metal single atoms anchored on NC materials (M ISAS/NC, where M refers to Mo and Sn). This strategy is readily scalable and the as-prepared sintering-resistant M ISAS/NC catalysts hold great potential in high-temperature applications.
中文翻译:
通过气体传输方法将氧化铜(I)本体直接转化为孤立的单原子铜位点催化剂。
单原子金属催化剂引起了极大的关注,但是将廉价且容易获得的块状金属氧化物直接转化为单原子仍然是巨大的挑战。在这里,我们报告了一种简便而通用的气体传输策略,以克水平合成孤立的单原子铜位点(Cu ISAS / NC)催化剂。商用氧化铜(I)粉末在接近熔化温度(1500 K)处升华为移动蒸气,随后可被富缺陷的氮掺杂碳(NC)捕集并还原,从而形成分离的铜位点催化剂。令人惊讶的是,在1270 K以上获得的这种热稳定的Cu ISAS / NC具有优异的氧还原性能,相对于RHE而言,其半波电势记录为0.92 V(相对于其他Cu基电催化剂而言)。通过改变金属氧化物的前体,我们证明了锚定在NC材料(M ISAS / NC,其中M表示Mo和Sn)上的不同金属单原子的通用合成。该策略易于扩展,并且所制备的耐烧结M ISAS / NC催化剂在高温应用中具有巨大潜力。