Active hydrogen boosts electrochemical nitrate reduction to ammonia

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Дек. 27, 2022

Electrochemical nitrate reduction to ammonia is a promising alternative strategy the traditional Haber-Bosch process but suffers from low Faradaic efficiency and limited yield due sluggish multi-electron/proton-involved steps. Herein, we report typical hollow cobalt phosphide nanosphere electrocatalyst assembled on self-supported carbon nanosheet array synthesized with confinement that exhibits an extremely high rate of 8.47 mmol h

Язык: Английский

---

Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120010 - e9120010

Опубликована: Май 30, 2022

To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals minimal carbon emissions. The background of such N-cycles, as fixation, ammonia oxidation, nitrate reduction, is briefly introduced here. discussion emerging nanostructures in various conversion reactions focused on architecture/compositional design, electrochemical performances, reaction mechanisms, instructive tests. Energy device advancements for achieving more functions well in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed less discussed C–N coupling summarized. We classify inorganic sources that each other under an applied voltage into three types, namely, abundant nitrogen, toxic (nitrite), oxides, useful compounds ammonia, hydrazine, hydroxylamine, goal providing critical insights strategies facilitate development our circular economy.

Язык: Английский

---

Advances in ammonia electrosynthesis from ambient nitrate/nitrite reduction

Chem, Год журнала: 2023, Номер 9(7), С. 1768 - 1827

Опубликована: Июнь 21, 2023

Язык: Английский

---

Efficient Ammonia Electrosynthesis and Energy Conversion through a Zn‐Nitrate Battery by Iron Doping Engineered Nickel Phosphide Catalyst

Advanced Energy Materials, Год журнала: 2022, Номер 12(13)

Опубликована: Фев. 9, 2022

Abstract The electrocatalytic nitrate reduction reaction (NO 3 ‐RR) to ammonia (NH ) offers a promising alternative approach for NH production and nitrate‐based voltaic cells which can deliver both electricity as products, are also highly attractive. However, nitrate‐to‐NH conversion involves proton‐assisted multiple‐electron transfer process with considerable kinetic barrier, underlying the need efficient catalysts NO – RR. A Zn‐nitrate battery is reported enable “killing three birds one stone” strategy energy supply, removal of pollutants iron doped nickel phosphide (Fe/Ni 2 P) RR catalyst electrode. Iron doping induces downshift d‐band center Ni atoms Fermi level, allowing optimization Gibbs free energies intermediates. Fe/Ni P exhibits 94.3% Faradaic efficiency (FE) nearly 100% at –0.4 V vs. reversible hydrogen electrode (RHE). Further applying this electrocatalyst cathode material, novel power density 3.25 mW cm –2 FE 85.0% production. This work enriches application Zn‐based batteries in field electrocatalysis highlights promise bimetal

Язык: Английский

---

Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Июнь 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Язык: Английский

---

Ambient Ammonia Synthesis via Electrochemical Reduction of Nitrate Enabled by NiCo₂O₄ Nanowire Array

Small, Год журнала: 2022, Номер 18(13)

Опубликована: Фев. 10, 2022

NiCo2 O4 nanowire array on carbon cloth (NiCo2 /CC) is proposed as a highly active electrocatalyst for ambient nitrate (NO3- ) reduction to ammonia (NH3 ). In 0.1 m NaOH solution with NaNO3 , such /CC achieves high Faradic efficiency of 99.0% and large NH3 yield up 973.2 µmol h-1 cm-2 . The superior catalytic activity comes from its half-metal feature optimized adsorption energy due the existence Ni in crystal structure. A Zn-NO3- battery cathode also shows record-high performance.

Язык: Английский

---

Pulsed Nitrate-to-Ammonia Electroreduction Facilitated by Tandem Catalysis of Nitrite Intermediates

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(11), С. 6471 - 6479

Опубликована: Март 10, 2023

Electroreduction of nitrate to ammonia offers a promising pathway for nutrient recycling and recovery from wastewater with energy environmental sustainability. There have been considerable efforts on the regulation reaction pathways facilitate nitrate-to-ammonia conversion over competing hydrogen evolution but only limited success. Here, we report Cu single-atom gel (Cu SAG) electrocatalyst that produces NH3 both nitrite under neutral conditions. Given unique mechanism NO2- activation SAGs spatial confinement strengthened kinetics, pulse electrolysis strategy is presented cascade accumulation intermediates during NO3- reduction prohibited competition reaction, thus substantially enhancing Faradaic efficiency yield rate production compared constant potential electrolysis. This work underlines cooperative approach three-dimensional (3D) framework structures highly efficient enabled by tandem catalysis unfavorable intermediates.

Язык: Английский

---

Electrocatalytic nitrate reduction to ammonia on defective Au1Cu (111) single-atom alloys

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 310, С. 121346 - 121346

Опубликована: Март 26, 2022

Язык: Английский

---

Electrocatalytic conversion of nitrate waste into ammonia: a review

Environmental Chemistry Letters, Год журнала: 2022, Номер 20(5), С. 2929 - 2949

Опубликована: Июль 9, 2022

Язык: Английский

---

Intermetallic Single-Atom Alloy In–Pd Bimetallene for Neutral Electrosynthesis of Ammonia from Nitrate

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(25), С. 13957 - 13967

Опубликована: Июнь 19, 2023

Harvesting recyclable ammonia (NH3) from the electrocatalytic reduction of nitrate (NO3RR) offers a sustainable strategy to close ecological nitrogen cycle nitration contamination in an energy-efficient and environmentally friendly manner. The emerging intermetallic single-atom alloys (ISAAs) are recognized achieve highest site density single atoms by isolating contiguous metal into sites stabilized another within structure, which holds promise couple catalytic benefits nanocrystals catalysts for promoting NO3RR. Herein, ISAA In-Pd bimetallene, Pd isolated surrounding In atoms, is reported boost neutral NO3RR with NH3 Faradaic efficiency (FE) 87.2%, yield rate 28.06 mg h-1 mgPd-1, exceptional stability increased activity/selectivity over 100 h 20 cycles. structure induces substantially diminished overlap d-orbitals narrowed p-d hybridization In-p Pd-d states around Fermi level, resulting stronger NO3- adsorption depressed energy barrier potential-determining step Further integrating catalyst Zn-NO3- flow battery as cathode delivers power 12.64 mW cm-2 FE 93.4% production.

Язык: Английский

---