Synergistic electroreduction of carbon dioxide to carbon monoxide on bimetallic layered conjugated metal-organic frameworks.
Haixia ZhongMahdi Ghorbani-AslKhoa Hoang LyJichao ZhangJin GeMingchao WangZhongquan LiaoDenys MakarovEhrenfried ZschechEike BrunnerInez M WeidingerJian ZhangArkady V KrasheninnikovStefan KaskelRenhao DongXinliang FengPublished in: Nature communications (2020)
Highly effective electrocatalysts promoting CO2 reduction reaction (CO2RR) is extremely desirable to produce value-added chemicals/fuels while addressing current environmental challenges. Herein, we develop a layer-stacked, bimetallic two-dimensional conjugated metal-organic framework (2D c-MOF) with copper-phthalocyanine as ligand (CuN4) and zinc-bis(dihydroxy) complex (ZnO4) as linkage (PcCu-O8-Zn). The PcCu-O8-Zn exhibits high CO selectivity of 88%, turnover frequency of 0.39 s-1 and long-term durability (>10 h), surpassing thus by far reported MOF-based electrocatalysts. The molar H2/CO ratio (1:7 to 4:1) can be tuned by varying metal centers and applied potential, making 2D c-MOFs highly relevant for syngas industry applications. The contrast experiments combined with operando spectroelectrochemistry and theoretical calculation unveil a synergistic catalytic mechanism; ZnO4 complexes act as CO2RR catalytic sites while CuN4 centers promote the protonation of adsorbed CO2 during CO2RR. This work offers a strategy on developing bimetallic MOF electrocatalysts for synergistically catalyzing CO2RR toward syngas synthesis.
Keyphrases
- metal organic framework
- carbon dioxide
- photodynamic therapy
- reduced graphene oxide
- room temperature
- quantum dots
- heavy metals
- cancer therapy
- oxide nanoparticles
- magnetic resonance
- human health
- ionic liquid
- genome wide
- bone mineral density
- magnetic resonance imaging
- hepatitis c virus
- body composition
- contrast enhanced
- crystal structure
- highly efficient
- dna methylation
- postmenopausal women
- human immunodeficiency virus
- high density