Solid-Phase Upcycling Toward the Production of Ultrahigh-Loading Single-Atom Catalysts

IF 13.7 Q1 CHEMISTRY, MULTIDISCIPLINARY

Aggregate (Hoboken, N.J.) Pub Date : 2025-05-19 DOI:10.1002/agt2.70052

Guanwu Lian, Zefan Du, Yifan Wang, Yelan Xiao, Mengyao Su, Chao Wu, Yucong Huang, Yuansheng Lin, Jingjing Xiong, Yichen Chen, Shibo Xi, Wenguang Tu, Zhigang Zou, Zhongxin Chen

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Abstract

The recovery of valuable transition metals from deactivated catalysts is crucial for alleviating the challenges of resource scarcity and environmental pollution. Guided by AI-powered big data analysis, we identified an important research gap in the sustainable recovery of early transition metals and proposed a solid-phase upcycling strategy to transform waste catalysts into highly valuable single-atom catalysts (SACs). This involves a heat-induced redispersion of metal aggregates into single atoms on the polycrystalline carbon nitride (PCN) support, producing highly active M₁-PCN SACs up to 20 wt% (M = Cu, Fe, Co, and Ni). Subsequent techno-economic analysis confirms a two-thirds reduction in production cost and greenhouse gas emissions compared to conventional hydrometallurgical and pyrometallurgical processes, thus paving a new path in the development of sustainable technologies for metal recovery.

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固相升级循环制备超高负载单原子催化剂

从失活催化剂中回收有价值的过渡金属对于缓解资源短缺和环境污染的挑战至关重要。在人工智能驱动的大数据分析的指导下，我们发现了早期过渡金属可持续回收的重要研究空白，并提出了将废弃催化剂转化为高价值单原子催化剂（SACs）的固相升级回收策略。这涉及到金属聚集体在多晶碳氮（PCN）载体上的热诱导再分散成单原子，产生高达20% wt%的高活性M1-PCN SACs （M = Cu, Fe， Co和Ni）。随后的技术经济分析证实，与传统的湿法冶金和火法冶金工艺相比，生产成本和温室气体排放降低了三分之二，从而为可持续金属回收技术的发展铺平了新的道路。

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