Iron-Single Sites Confined by Graphene Lattice for Ammonia Synthesis under Mild Conditions

被引：19

作者：

Chen, Ziquan ^{[1
,2
]}

Ye, Yihan ^{[1
,2
]}

Peng, Tao ^{[1
,3
]}

Wu, Chenxin ^{[4
]}

Li, Haiyang ^{[4
]}

Pan, Xiulian ^{[1
]}

Bao, Xinhe ^{[1
]}

机构：

[1] Chinese Acad Sci, State Key Lab Catalysis, Dalian Inst Chem Phys, Dalian 116023, Peoples R China

[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

[3] Univ Sci & Technol China, Hefei 230026, Peoples R China

[4] Chinese Acad Sci, CAS Key Lab Separat Sci Analyt Chem, Dalian Inst Chem Phys, Dalian 116023, Peoples R China

来源：

ACS CATALYSIS | 2023年 / 13卷 / 21期

关键词：

nanoconfined catalysis; single-site catalysis; biomimetic catalysis; ammonia synthesis; associativemechanism; OXYGEN REDUCTION; RAMAN-SPECTRA; NITROGEN; SPECTROSCOPY; CARBON; CONVERSION; CATALYSTS; COFACTOR; BAND; ION;

D O I：

10.1021/acscatal.3c03108

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Development of ammonia synthesis catalysts under mild conditions is highly desirable for carbon neutrality. Herein, we report that an iron-single-site catalyst confined within the graphene lattice derived from ball milling of iron phthalocyanine with graphene and promoted by alkali metal enables ammonia synthesis below 200 C-degrees and atmospheric pressure. It exhibits an activity of 1.1 mu mol(NH3) gc (-1) h(-1) at 150( degrees)C and 10.3 mu mol(NH3) gc( -1) h(-1) at 190( degrees)C, whereas no activity is detected over a physical mixture of iron phthalocyanine and graphene. X-ray absorption fine structure analysis and( 15)N(2)-H-2 periodic switching experiments revealed that iron-single sites are stabilized as FeN4 sites within the graphene lattice and evolve to FeN3 as the active sites during the reaction. N-2 transformation to NH3 follows an associative mechanism, evidenced by the presence of N2H2+ and N2H3 (+) detected by TOF-MS. These findings could guide further development of more active catalysts for mild ammonia synthesis.

引用

页码：14385 / 14394

页数：10

共 57 条

[1] Enabling electrochemical reduction of nitrogen to ammonia at ambient conditions through rational catalyst design [J].