Ambient nitrogen reduction cycle using a hybrid inorganic–biological system

Liu, Chong; Sakimoto, Kelsey K.; Colón, Brendan; Silver, Pamela A.; Nocera, Daniel G.

doi:10.1073/pnas.1706371114

Cited by 192 publications

(240 citation statements)

References 41 publications

Supporting

Mentioning

220

Contrasting

Order By: Relevance

“…As one of the extremely common industrial chemicals, NH 3 is widely used in various fields such as agriculture and industry . In addition to the biosynthesis of NH 3 , industrially, NH 3 is primarily generated from N 2 through the Haber–Bosch process, yielding roughly 500 million tons per year with an Fe‐ or Ru‐based catalyst . Such a process, however, operates at high temperatures (400–500 °C) and pressures (200–250 atm), accounting for ≈2 % of the world's energy consumption and releasing large amounts of CO 2 annually .…”

Section: Figurementioning

confidence: 99%

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N₂ Fixation to NH₃ under Ambient Conditions

Huang

Cao

et al. 2019

Chemistry A European J

View full text Add to dashboard Cite

Currently, NH3 production primarily depends on the Haber–Bosch process, which operates at elevated temperatures and pressures and leads to serious CO2 emissions. Electrocatalytic N2 reduction offers an environmentally benign approach for the sustainable synthesis of NH3 under ambient conditions. This work reports the development of biomass‐derived amorphous oxygen‐doped carbon nanosheet (O−CN) using tannin as the precursor. As a metal‐free electrocatalyst for N2‐to‐NH3 conversion, such O−CN shows high catalytic performances, achieving a large NH3 yield of 20.15 μg h−1 mg−1cat. and a high Faradic efficiency of 4.97 % at −0.6 V vs. reversible hydrogen electrode (RHE) in 0.1 m HCl at ambient conditions. Remarkably, it also exhibits high electrochemical selectivity and durability.

show abstract

Section: Figurementioning

confidence: 99%

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N₂ Fixation to NH₃ under Ambient Conditions

Huang

Cao

et al. 2019

Chemistry A European J

View full text Add to dashboard Cite

show abstract

“…Comprehensive solar-to-chemical production has been investigated with bioinorganic hybrid systems including semiconductor-conjugated hydrogenases for biohydrogen production (3–5), long wavelength-absorbing nanomaterials integrated into plants for enhanced photosynthetic efficiency (6), and photoelectrodes coupled with whole cells for hydrogenation reactions (7), and atmospheric CO 2 and N 2 fixation (8–11). …”

mentioning

confidence: 99%

Light-driven fine chemical production in yeast biohybrids

Guo

Suástegui

Sakimoto

et al. 2018

Science

Self Cite

291

256

View full text Add to dashboard Cite

Inorganic-biological hybrid systems have potential to be sustainable, efficient, and versatile chemical synthesis platforms by integrating the light-harvesting properties of semiconductors with the synthetic potential of biological cells. We have developed a modular bioinorganic hybrid platform that consists of highly efficient light-harvesting indium phosphide nanoparticles and genetically engineered Saccharomyces cerevisiae: a workhorse microorganism in biomanufacturing. The yeast harvests photo-generated electrons from the illuminated nanoparticles and uses them for the cytosolic regeneration of redox cofactors. This enables the decoupling of biosynthesis and cofactor regeneration, facilitating a carbon- and energy-efficient production of the metabolite shikimic acid – a common precursor for several drugs and fine chemicals. Our work provides a platform for the rational design of biohybrids for efficient biomanufacturing processes with higher complexity and functionality.

show abstract

“…Hydrogen may be used directly as a fuel (3,4) or converted into a liquid fuel with its combination with carbon dioxide via inorganic (5) or hybrid biological-inorganic catalysts (6)(7)(8). In addition, renewable hydrogen may be used to derive other energy-intensive products (9) such as ammonia for fertilization (10). Although an atomically simple conversion, the bond rearrangement of two water molecules to hydrogen and oxygen is chemically complex.…”

mentioning

confidence: 99%

Self-healing catalysis in water

Costentin

Nocera

2017

Proc. Natl. Acad. Sci. U.S.A.

Self Cite

123

View full text Add to dashboard Cite

Principles for designing self-healing water-splitting catalysts are presented together with a formal kinetics model to account for the key chemical steps needed for self-healing. Self-healing may be realized if the catalysts are able to self-assemble at applied potentials less than that needed for catalyst turnover. Solution pH provides a convenient handle for controlling the potential of these two processes, as demonstrated for the cobalt phosphate (CoP i ) watersplitting catalyst. For Co 2+ ion that appears in solution due to leaching from the catalyst during turnover, a quantitative description for the kinetics of the redeposition of the ion during the self-healing process has been derived. The model reveals that OER activity of CoP i occurs with negligible film dissolution in neutral pH for typical cell geometries and buffer concentrations. solar energy | water splitting | renewable energy storage | self-healing catalysis | cobalt phosphate W ater is a desirable medium for storing solar energy. Chargeseparated states generated by solar capture in semiconductors may be transferred directly or indirectly to catalysts, which rearrange the chemical bonds of water to produce the high-energy products of oxygen and hydrogen (1, 2). Hydrogen may be used directly as a fuel (3, 4) or converted into a liquid fuel with its combination with carbon dioxide via inorganic (5) or hybrid biological-inorganic catalysts (6-8). In addition, renewable hydrogen may be used to derive other energy-intensive products (9) such as ammonia for fertilization (10). Although an atomically simple conversion, the bond rearrangement of two water molecules to hydrogen and oxygen is chemically complex. The reaction encompasses a four-electron process, and this multielectron inventory must be coupled intimately to protons (11) to avoid the high-energy intermediates summarized on the Frost diagram of water ( Fig. 1). Most water-splitting catalysis is performed in concentrated base (12). However, in contradistinction to the harsh conditions of basic water, the ease and simplicity of interfacing catalysts to semiconducting materials in fabricated devices such as buried junctions [e.g., the artificial leaf (13,14)] is facilitated when neutral or near-neutral water is used, which also engenders greater materials stability and lessened liability for the implementation of new technologies. For these reasons, earth-abundant materials for water splitting at neutral and near-neutral conditions is now generally being adopted as a preferred approach for achieving direct photoelectrochemical energy conversion processes (15). Nonetheless, the use of pure water is insufficient to meet future global energy needs. Growth in energy during this century is projected to be driven by the urgent needs of emerging and low-income countries that currently lack access to reliable energy (16). Achieving the decarbonization needed to address climate change in the developing world has provided an imperative for the development of a distributed renewable energy infrastructure...

show abstract

Ambient nitrogen reduction cycle using a hybrid inorganic–biological system

Cited by 192 publications

References 41 publications

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N₂ Fixation to NH₃ under Ambient Conditions

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N₂ Fixation to NH₃ under Ambient Conditions

Light-driven fine chemical production in yeast biohybrids

Self-healing catalysis in water

Contact Info

Product

Resources

About

Ambient nitrogen reduction cycle using a hybrid inorganic–biological system

Cited by 192 publications

References 41 publications

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N2 Fixation to NH3 under Ambient Conditions

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N2 Fixation to NH3 under Ambient Conditions

Light-driven fine chemical production in yeast biohybrids

Self-healing catalysis in water

Contact Info

Product

Resources

About

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N₂ Fixation to NH₃ under Ambient Conditions

A Biomass‐Derived Carbon‐Based Electrocatalyst for Efficient N₂ Fixation to NH₃ under Ambient Conditions