It is highly desirable to develop industrially scalable methods to produce defect-free graphene to meet the requirement of graphene from lab to commercial applications. In this paper, a ball-milling in series with a shear-mixing exfoliation technique in supercritical CO₂ was developed. Graphite was pretreated by ball-milling in supercritical CO₂, and the exfoliated sheets with smaller lateral sizes and numerous crevices on their edges were elutriated into a shear-mixing vessel by supercritical CO₂ simultaneously to inhibit over crushing. Whereafter, the freshly exfoliated sheets with crevices were further exfoliated into few-layer graphene without aggregation. 90% of the obtained graphene was less than five layers, and the processing capacity of 40 g for one batch increased 40–100 times compared with the previously reported method. The electrical conductivity of 3.25 × 10⁵ S/m of the flexible graphene film on PVDF substrate demonstrates the excellent electrical performance of the obtained graphene.

非常需要开发工业上可扩展的方法来生产无缺陷的石墨烯，以满足从实验室到商业应用的石墨烯需求。在本文中，开发了一种在超临界 CO ₂中采用剪切混合剥离技术的串联球磨机。石墨在超临界 CO _{2 中}通过球磨预处理，横向尺寸较小且边缘有大量裂缝的剥离片被超临界 CO ₂淘洗到剪切混合容器中同时抑制过粉碎。此后，新剥离的带有裂缝的薄片被进一步剥离成少层石墨烯而没有聚集。得到的石墨烯90%不到五层，与之前报道的方法相比，一批40g的处理能力提高了40-100倍。PVDF 基板上柔性石墨烯薄膜的电导率为 3.25 × 10 ⁵ S/m，表明所获得的石墨烯具有优异的电学性能。