Prospects and Challenges for Solar Fertilizers

Comer, Benjamin M.; Fuentes, Porfirio A.; Dimkpa, Christian O.; Liu, Yu-Hsuan; Fernández, Carlos A.; Arora, Pratham; Park, Jongwoo; Singh, Upendra; Hatzell, Marta C.; Medford, Andrew J.

doi:10.1016/j.joule.2019.05.001

Cited by 200 publications

(192 citation statements)

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“…NH 3 has been synthesized through the reaction of hydrogen and nitrogen under high temperature and high pressure, namely the Haber–Bosch method . The production, purification, and compression of hydrogen and nitrogen are highly energy‐intensive . Moreover, the preparation of hydrogen via the reforming of natural gas is accompanied by the emission of huge amounts of greenhouse gas .…”

Section: Figurementioning

confidence: 99%

“…[9][10][11] The production, purification, and compression of hydrogen and nitrogen are highly energyintensive. [12,13] Moreover, the preparation of hydrogen via the reforming of natural gas is accompanied by the emission of huge amounts of greenhouse gas. [14] Thus, using water as a hydrogen source to prepare ammonia through electrocatalytic and photo(electro)catalytic nitrogen reduction has attracted increasing attention.…”

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Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

et al. 2020

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Unveiling the active phase of catalytic materials under reaction conditions is important for the construction of efficient electrocatalysts for selective nitrate reduction to ammonia. The origin of the prominent activity enhancement for CuO (Faradaic efficiency: 95.8 %, Selectivity: 81.2 %) toward selective nitrate electroreduction to ammonia was probed. 15N isotope labeling experiments showed that ammonia originated from nitrate reduction. 1H NMR spectroscopy and colorimetric methods were performed to quantify ammonia. In situ Raman and ex situ experiments revealed that CuO was electrochemically converted into Cu/Cu2O, which serves as an active phase. The combined results of online differential electrochemical mass spectrometry (DEMS) and DFT calculations demonstrated that the electron transfer from Cu2O to Cu at the interface could facilitate the formation of *NOH intermediate and suppress the hydrogen evolution reaction, leading to high selectivity and Faradaic efficiency.

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Section: Figurementioning

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Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

et al. 2020

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“…The reactive forms of nitrogen, such as ammonia (NH 3 ) [5,6], hydrazine (N 2 H 4 ) [7], nitride oxides (NO x ) [8], nitrite (NO 2 − ) and nitrate (NO 3 − ) [9], are crucial for the utilization of the nitrogen element. Particularly, ammonia, with an annual output of~200 million metric tons, has been widely used as a raw material for agricultural fertilizers and industrial productions [10,11]. Additionally, NH 3 is expected to serve as next-generation green energy carriers due to its high energy density, low liquefying pressure, small air-fuel ratio and no carbon dioxide emission [12,13].…”

Section: Introductionmentioning

confidence: 99%

Promoting selective electroreduction of nitrates to ammonia over electron-deficient Co modulated by rectifying Schottky contacts

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Developing efficient electrocatalysts for selective nitrate contamination reduction into value-added ammonia is significant. Here, heterostructured Co/CoO nanosheet arrays (Co/CoO NSAs) exhibited excellent Faradaic efficiency (93.8%) and selectivity (91.2%) for nitrate electroreduction to ammonia, greatly outperforming Co NSAs. 15 N isotope labeling experiments and 1 H nuclear magnetic resonance (NMR) quantitative testing methods confirmed the origin of the produced ammonia. Electrochemical in situ Fourier transform infrared (FTIR) spectroscopy, online differential electrochemical mass spectrometry (DEMS) data and density functional theory (DFT) results revealed that the superior performances arose from the electron deficiency of Co induced by the rectifying Schottky contact in the Co/CoO heterostructures. The electron transfer from Co to CoO at the interface could not only suppress the competitive hydrogen evolution reaction, but also increase energy barriers for by-products, thus leading to high Faradaic efficiency and selectivity of ammonia.

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“…Theoretical calculations are of great significance to the selection of catalysts and the understanding of reaction mechanisms. Medford and co-workers have carried out significant and pioneering research on this topic, developing fundamental understanding of the molecular-scale processes that underlie the important and potentially transformative N 2 and CO 2 reduction processes [37][38][39][40] . Inspired by their instructive theory that the carbon radicals on the catalyst surface can interact strongly with N 2 molecules to facilitate the catalytic process 33 , possible mechanisms for C-N bond formation via the thermodynamic spontaneous reaction between *N=N* (the asterisks here indicate the side-on sorption of N 2 ) and CO were proposed, and the subsequent hydrogenations enable the generation of urea.…”

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Coupling N2 and CO2 in H2O to synthesize urea under ambient conditions

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© 2020, The Author(s), under exclusive licence to Springer Nature Limited. The use of nitrogen fertilizers has been estimated to have supported 27% of the world's population over the past century. Urea (CO(NH2)2) is conventionally synthesized through two consecutive industrial processes, N2 + H2 → NH3 followed by NH3 + CO2 → urea. Both reactions operate under harsh conditions and consume more than 2% of the world's energy. Urea synthesis consumes approximately 80% of the NH3 produced globally. Here we directly coupled N2 and CO2 in H2O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO2 nanosheets. This coupling reaction occurs through the formation of C-N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g-1 h-1 and corresponding Faradic efficiency of 8.92% were measured at-0.4 V versus reversible hydrogen electrode.

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Prospects and Challenges for Solar Fertilizers

Cited by 200 publications

References 133 publications

Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Promoting selective electroreduction of nitrates to ammonia over electron-deficient Co modulated by rectifying Schottky contacts

Coupling N2 and CO2 in H2O to synthesize urea under ambient conditions

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