Confined Fe-Cu Clusters as Sub-Nanometer Reactors for Efficiently Regulating the Electrochemical Nitrogen Reduction Reaction

Wang Xiaowei; Qiu Siyao; Feng Jianmin; Tong Yueyu; Zhou Fengling; Li Qinye; Song Li; Chen Shuangming; Su Panpan; Ye Sheng; Hou Feng; Dou Shi Xue; Liu Hua Kun; Lu Gao Qing (Max); Sun Chenghua; Liu Jian; Liang Ji; Wu Kuang-Hsu

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Confined Fe-Cu Clusters as Sub-Nanometer Reactors for Efficiently Regulating the Electrochemical Nitrogen Reduction Reaction

机译：限制Fe-Cu簇作为亚纳米反应器，用于有效调节电化学氮还原反应

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Electrochemical nitrogen reduction reaction (NRR) over nonprecious-metal and single-atom catalysts has received increasing attention as a sustainable strategy to synthesize ammonia. However, the atomic-scale regulation of such active sites for NRR catalysis remains challenging because of the large distance between them, which significantly weakens their cooperation. Herein, the utilization of regular surface cavities with unique microenvironment on graphitic carbon nitride as "subnano reactors" to precisely confine multiple Fe and Cu atoms for NRR electrocatalysis is reported. The synergy of Fe and Cu atoms in such confined subnano space provides significantly enhanced NRR performance, with nearly doubles ammonia yield and 54%-increased Faradic efficiency up to 34%, comparing with the single-metal counterparts. First principle simulation reveals this synergistic effect originates from the unique Fe-Cu coordination, which effectively modifies the N(2)absorption, improves electron transfer, and offers extra redox couples for NRR. This work thus provides new strategies of manipulating catalysts active centers at the sub-nanometer scale.

机译：在非牙科金属和单原子催化剂上的电化学氮还原反应（NRR）已接受越来越关注，作为合成氨的可持续策略。然而，由于它们之间的距离很大，因此NRR催化的这种活性位点的原子级调节仍然具有挑战性，这显着削弱了合作。这里，报道了在石墨碳氮化物上具有独特的微环境的常规表面腔作为“亚诺反应器”，以精确限制NRR电闭合的“亚诺反应器”。 Fe和Cu原子在如此密闭的亚网上空间中的协同作用提供了显着提高的NRR性能，几乎双打氨产率和54％ - 增加的法拉米效率高达34％，比较单金属对应物。第一个原理仿真显示出该协同效应来自独特的Fe-Cu协调，这有效地改变了N（2）吸收，改善了电子转移，并为NRR提供了额外的氧化还原耦合。因此，这项工作提供了在子纳米级上操纵催化剂活性中心的新策略。

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来源
《Advanced Materials》 |2020年第40期|2004382.1-2004382.9|共9页
作者
Wang Xiaowei; Qiu Siyao; Feng Jianmin; Tong Yueyu; Zhou Fengling; Li Qinye; Song Li; Chen Shuangming; Su Panpan; Ye Sheng; Hou Feng; Dou Shi Xue; Liu Hua Kun; Lu Gao Qing (Max); Sun Chenghua; Liu Jian; Liang Ji; Wu Kuang-Hsu;
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作者单位

Tianjin Univ Sch Mat Sci & Engn Key Lab Adv Ceram & Machining Technol Minist Educ Tianjin 300350 Peoples R China|Tianjin Normal Univ Coll Phys & Mat Sci Appl Phys Dept 393 Binshui West Rd Tianjin 300387 Peoples R China|Univ Wollongong Inst Superconducting & Elect Mat Wollongong NSW 2522 Australia;

Dongguan Univ Technol Sci & Technol Innovat Inst Dongguan 523000 Peoples R China;

Tianjin Normal Univ Coll Phys & Mat Sci Appl Phys Dept 393 Binshui West Rd Tianjin 300387 Peoples R China;

Univ Wollongong Inst Superconducting & Elect Mat Wollongong NSW 2522 Australia;

Dongguan Univ Technol Sci & Technol Innovat Inst Dongguan 523000 Peoples R China;

Swinburne Univ Technol Dept Chem & Biotechnol Hawthorn Vic 3122 Australia|Swinburne Univ Technol Ctr Translat Atomat FSET Hawthorn Vic 3122 Australia;

Univ Sci & Technol China CAS Ctr Excellence Nanosci Natl Synchrotron Radiat Lab Hefei 230029 Anhui Peoples R China;

Univ Sci & Technol China CAS Ctr Excellence Nanosci Natl Synchrotron Radiat Lab Hefei 230029 Anhui Peoples R China;

Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis 457 Zhongshan Rd Dalian 116023 Peoples R China;

Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis 457 Zhongshan Rd Dalian 116023 Peoples R China;

Tianjin Univ Sch Mat Sci & Engn Key Lab Adv Ceram & Machining Technol Minist Educ Tianjin 300350 Peoples R China;

Univ Wollongong Inst Superconducting & Elect Mat Wollongong NSW 2522 Australia;

Univ Wollongong Inst Superconducting & Elect Mat Wollongong NSW 2522 Australia;

Univ Surrey DICP Surrey Joint Ctr Future Mat Dept Chem & Proc Engn Guildford GU2 7XH Surrey England|Univ Surrey Adv Technol Inst Guildford GU2 7XH Surrey England;

Swinburne Univ Technol Dept Chem & Biotechnol Hawthorn Vic 3122 Australia|Swinburne Univ Technol Ctr Translat Atomat FSET Hawthorn Vic 3122 Australia;

Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis 457 Zhongshan Rd Dalian 116023 Peoples R China|Univ Surrey DICP Surrey Joint Ctr Future Mat Dept Chem & Proc Engn Guildford GU2 7XH Surrey England|Univ Surrey Adv Technol Inst Guildford GU2 7XH Surrey England;

Tianjin Univ Sch Mat Sci & Engn Key Lab Adv Ceram & Machining Technol Minist Educ Tianjin 300350 Peoples R China|Univ Wollongong Inst Superconducting & Elect Mat Wollongong NSW 2522 Australia;

Univ New South Wales Sch Chem Engn Sydney NSW 2052 Australia;

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正文语种 eng
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关键词
atomic clusters; electrochemical nitrogen fixation; graphitic carbon nitride; sub-nanometer reactors; synergistic effect;

机译：原子簇;电化学氮固定;石墨碳氮化物;亚纳米反应器;协同效应;

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Confined Fe-Cu Clusters as Sub-Nanometer Reactors for Efficiently Regulating the Electrochemical Nitrogen Reduction Reaction

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