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通过将还原氧化石墨烯和非晶态碳与超细 MgO 纳米晶集成的分级纳米复合材料增强 CO 捕获。

Hierarchical Nanocomposite by the Integration of Reduced Graphene Oxide and Amorphous Carbon with Ultrafine MgO Nanocrystallites for Enhanced CO Capture.

机构信息

Department of Chemical and Biomolecular Engineering, Faculty of Engineering, National University of Singapore , 10 Kent Ridge Crescent, 119260 Singapore.

出版信息

Environ Sci Technol. 2017 Nov 7;51(21):12998-13007. doi: 10.1021/acs.est.7b03308. Epub 2017 Oct 17.

Abstract

Exploring efficient and low-cost solid sorbents is essential for carbon capture and storage. Herein, a novel class of high-performance CO adsorbent (rGO@MgO/C) is engineered based on the controllable integration of reduced graphene oxide (rGO), amorphous carbon, and MgO nanocrystallites. The optimized rGO@MgO/C nanocomposite exhibits remarkable CO capture capacity (up to 31.5 wt % at 27 °C, 1 bar CO, and 22.5 wt % under the simulated flue gas), fast sorption rate, and strong process durability. The enhanced capture capability of CO is the best among all of the MgO-based sorbents reported so far. The high performance of rGO@MgO/C nanocomposite can be ascribed to the hierarchical architecture and special physicochemical features, including the sheet-on-sheet sandwich-like structure, ultrathin nanosheets with abundant nanopores, large surface area, and highly dispersed ultrafine MgO nanocrystallites (ca. 3 nm in size), together with the rGO sheets and in situ generated amorphous carbon that serve as a dual carbon support and protectant system with which to prevent MgO nanocrystallites from agglomeration. In addition, the CO-uptake capacity at intermediate temperature (e.g., 350 °C) can be further improved threefold through alkali metal salt promotion treatment. This work provides a facile and effective strategy with which to engineer advanced graphene-based functional nanocomposites with rationally designed compositions and architectures for potential applications in the field of gas storage and separation.

摘要

探索高效且低成本的固体吸附剂对于碳捕获和封存至关重要。在此,基于可控整合还原氧化石墨烯(rGO)、无定形碳和 MgO 纳米晶,设计了一类新型高性能 CO 吸附剂(rGO@MgO/C)。优化后的 rGO@MgO/C 纳米复合材料表现出显著的 CO 捕获能力(在 27°C、1 巴 CO 和模拟烟道气下分别高达 31.5wt%和 22.5wt%)、快速吸附速率和强过程耐久性。CO 的增强捕获能力是迄今为止所有报道的基于 MgO 的吸附剂中最好的。rGO@MgO/C 纳米复合材料的高性能可归因于其分层结构和特殊的物理化学特性,包括片层对片层的夹层状结构、具有丰富纳米孔的超薄纳米片、大表面积和高度分散的超细 MgO 纳米晶(约 3nm 大小),以及 rGO 片和原位生成的无定形碳,它们作为双碳支撑和保护体系,防止 MgO 纳米晶团聚。此外,通过碱金属盐促进处理,可将中间温度(例如 350°C)下的 CO 吸收容量进一步提高三倍。这项工作为工程设计提供了一种简便有效的策略,可用于设计具有合理组成和结构的先进石墨烯基功能纳米复合材料,从而在气体储存和分离领域具有潜在应用。

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