Dataset Information

Engineering Spin States of Isolated Copper Species in a Metal-Organic Framework Improves Urea Electrosynthesis.

ABSTRACT: The catalytic activities are generally believed to be relevant to the electronic states of their active center, but understanding this relationship is usually difficult. Here, we design two types of catalysts for electrocatalytic urea via a coordination strategy in a metal-organic frameworks: Cu^III-HHTP and Cu^II-HHTP. Cu^III-HHTP exhibits an improved urea production rate of 7.78 mmol h^-1 g^-1 and an enhanced Faradaic efficiency of 23.09% at - 0.6 V vs. reversible hydrogen electrode, in sharp contrast to Cu^II-HHTP. Isolated Cu^III species with S = 0 spin ground state are demonstrated as the active center in Cu^III-HHTP, different from Cu^II with S = 1/2 in Cu^II-HHTP. We further demonstrate that isolated Cu^III with an empty [Formula: see text] orbital in Cu^III-HHTP experiences a single-electron migration path with a lower energy barrier in the C-N coupling process, while Cu^II with a single-spin state ([Formula: see text]) in Cu^II-HHTP undergoes a two-electron migration pathway.

SUBMITTER: Gao Y

PROVIDER: S-EPMC10284786 | biostudies-literature | 2023 Jun

REPOSITORIES: biostudies-literature

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Engineering Spin States of Isolated Copper Species in a Metal-Organic Framework Improves Urea Electrosynthesis.

Gao Yuhang Y Wang Jingnan J Yang Yijun Y Wang Jian J Zhang Chuang C Wang Xi X Yao Jiannian J

Nano-micro letters 20230621 1

The catalytic activities are generally believed to be relevant to the electronic states of their active center, but understanding this relationship is usually difficult. Here, we design two types of catalysts for electrocatalytic urea via a coordination strategy in a metal-organic frameworks: CuIII-HHTP and CuII-HHTP. CuIII-HHTP exhibits an improved urea production rate of 7.78 mmol h-1 g-1 and an enhanced Faradaic efficiency of 23.09% at - ...[more]

PMID: 37341868

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Project description:Pesticides are agrochemical compounds used to kill pests (insects, rodents, fungi, or unwanted plants), which are key to meet the world food demand. Regrettably, some important issues associated with their widespread/extensive use (contamination, bioaccumulation, and development of pest resistances) demand a reduction in the amount of pesticide applied in crop protection. Among the novel technologies used to combat the deterioration of our environment, metal-organic frameworks (MOFs) have emerged as innovative and promising materials in agroindustry since they possess several features (high porosity, functionalizable cavities, ecofriendly composition, etc.) that make them excellent candidates for the controlled release of pesticides. Moving toward a sustainable development, in this work, we originally describe the use of pesticides as building blocks for the MOF construction, leading to a new type of agricultural applied MOFs (or AgroMOFs). Particularly, we have prepared a novel 2D-MOF (namely, GR-MOF-7) based on the herbicide glufosinate and the widely used antibacterial and fungicide Cu2+. GR-MOF-7 crystallizes attaining a monoclinic P21/c space group, and the asymmetric unit is composed of one independent Cu2+ ion and one molecule of the Glu2- ligand. Considering the significant antibacterial activity of Cu-based compounds in agriculture, the potential combined bactericidal and herbicidal effect of GR-MOF-7 was investigated. GR-MOF-7 shows an important antibacterial activity against Staphylococcus aureus and Escherichia coli (involved in agricultural animal infections), improving the results obtained with its individual or even physical mixed precursors [glufosinate and Cu(NO3)2]. It is also an effective pesticide against germination and plant growth of the weed Raphanus sativus, an invasive species in berries and vines crops, demonstrating that the construction of MOFs based on herbicide and antibacterial/antifungal units is a promising strategy to achieve multifunctional agrochemicals. To the best of our knowledge, this first report on the synthesis of an MOF based on agrochemicals (what we have named AgroMOF) opens new ways on the safe and efficient MOF application in agriculture.

Dataset Information

Engineering Spin States of Isolated Copper Species in a Metal-Organic Framework Improves Urea Electrosynthesis.

Publications

Engineering Spin States of Isolated Copper Species in a Metal-Organic Framework Improves Urea Electrosynthesis.

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