首页|Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocat-alytic activity of carbon materials.However,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect struc-ture remains a challenging task.Herein,the intrinsic pentagon carbon sites that can favor electron over-flow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center calculations.To experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)via π-π interactions.The multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-ordered π electron delocalization system as conductive network.The defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40％,superior to the Pt reference(7.97％).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermedi-ates,thus enhancing the electrocatalytic activity of the catalyst.This work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich car-bon catalysts.

Defect engineeringPentagon carbonCarbon quantum dotsElectrocatalytic activityTriiodide reduction

Siyi Hou、Xuedan Song、Chang Yu、Jiangwei Chang、Yiwang Ding、Yingbin Liu、Xiubo Zhang、Weizhe Liu、Jieshan Qiu

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State Key Lab of Fine Chemicals,Liaoning Key Lab for Energy Materials and Chemical Engineering,Frontier Science Center for Smart Materials,School of Chemical Engineering,Dalian University of Technology,Dalian 116024,Liaoning,China

Liaoning Key Lab for Energy Materials and Chemical Engineering,Frontier Science Center for Smart Materials,School of Chemistry,Dalian University of Technology,Dalian 116024,Liaoning,China

State Key Laboratory of Chemical Resource Engineering,College of Chemical Engineering,Beijing University of Chemical Technology,Beijing 100029,China

National Natural Science Foundation of ChinaNational Key R&D Program of ChinaFundamental Research Funds for the Central Universities

220780522022YFB4101602DUT22LAB612

2024

10.1016/j.jechem.2024.03.034

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.95(8)