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Title: Ambient Electrosynthesis of Ammonia: Electrode Porosity and Composition Engineering

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [3];  [4];  [4];  [1];  [1]; ORCiD logo [5];  [6];  [7];  [3];  [8];  [8];  [9];  [10]; ORCiD logo [4]
  1. Nankai Univ., Tianjin (People's Republic of China)
  2. Univ. of Toronto, Toronto, ON (Canada); Soochow Univ., Jiangsu (People's Republic of China)
  3. The Chinese Academy of Sciences, Taiyuan (China)
  4. Univ. of Toronto, Toronto, ON (Canada)
  5. Temple Univ., Philadelphia, PA (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States)
  7. Northwest Normal Univ., Lanzhou (People's Republic of China)
  8. Soochow Univ., Jiangsu (People's Republic of China)
  9. Stockholm Univ., Stockholm (Sweden)
  10. UNSW Australia, Sydney, NSW (Australia)
+ Show Author Affiliations

Ammonia, a key precursor for fertilizer production, convenient hydrogen carrier, and emerging clean fuel, plays a pivotal role in sustaining life on Earth. Currently, the main route for NH3 synthesis is by the heterogeneous catalytic Haber–Bosch process (N2+3 H2→2 NH3), which proceeds under extreme conditions of temperature and pressure with a very large carbon footprint. Herein we report that a pristine nitrogen–doped nanoporous graphitic carbon membrane (NCM) can electrochemically convert N2 into NH3 in an acidic aqueous solution under ambient conditions. The Faradaic efficiency and rate of production of NH3 on the NCM electrode reach 5.2 % and 0.08 g m–2 h–1, respectively. Functionalization of the NCM with Au nanoparticles dramatically enhances these performance metrics to 22 % and 0.36 gm–2 h–1, respectively. In conclusion, as this system offers the potential to be scaled to industrial levels it is highly likely that it might displace the century-old Haber–Bosch process.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1476757
Report Number(s):
BNL-209144-2018-JAAM
Journal Information:
Angewandte Chemie (International Edition), Vol. 57, Issue 38; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 136 works
Citation information provided by
Web of Science

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Cited By (37)

Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion journal November 2019
Adsorbing and Activating N 2 on Heterogeneous Au–Fe 3 O 4 Nanoparticles for N 2 Fixation journal November 2019
Emerging Functional Porous Polymeric and Carbonaceous Materials for Environmental Treatment and Energy Storage journal November 2019
Carbon‐Based Metal‐Free Catalysts for Electrocatalytic Reduction of Nitrogen for Synthesis of Ammonia at Ambient Conditions journal January 2019
2D Electrocatalysts for Converting Earth‐Abundant Simple Molecules into Value‐Added Commodity Chemicals: Recent Progress and Perspectives journal October 2019
Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction journal January 2020
Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future journal September 2019
High Efficiency Electrochemical Nitrogen Fixation Achieved with a Lower Pressure Reaction System by Changing the Chemical Equilibrium journal September 2019
Ammonia Synthesis Under Ambient Conditions: Selective Electroreduction of Dinitrogen to Ammonia on Black Phosphorus Nanosheets journal January 2019
High Efficiency Electrochemical Nitrogen Fixation Achieved with a Lower Pressure Reaction System by Changing the Chemical Equilibrium journal September 2019
Ambient Electrochemical N 2 Reduction to NH 3 on Nitrogen and Phosphorus Co‐doped Porous Carbon with Trace Iron in Alkaline Electrolytes journal December 2019
Ambient Electrosynthesis of Ammonia on a Core–Shell‐Structured Au@CeO 2 Catalyst: Contribution of Oxygen Vacancies in CeO 2 journal March 2019
Advanced Non‐metallic Catalysts for Electrochemical Nitrogen Reduction under Ambient Conditions journal July 2019
Amorphous Sn/Crystalline SnS 2 Nanosheets via In Situ Electrochemical Reduction Methodology for Highly Efficient Ambient N 2 Fixation journal August 2019
S‐Doped Carbon Nanospheres: An Efficient Electrocatalyst toward Artificial N 2 Fixation to NH 3 journal October 2018
Advances in Electrocatalytic N 2 Reduction—Strategies to Tackle the Selectivity Challenge journal October 2018
Recent Progress on Electrocatalyst and Photocatalyst Design for Nitrogen Reduction journal October 2018
Atomically Dispersed Single Ni Site Catalysts for Nitrogen Reduction toward Electrochemical Ammonia Synthesis Using N 2 and H 2 O journal February 2020
3D Hierarchical Porous Graphene-Based Energy Materials: Synthesis, Functionalization, and Application in Energy Storage and Conversion journal March 2019
A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements journal May 2019
Materials for electrochemical ammonia synthesis journal January 2019
Defect engineering in earth-abundant electrocatalysts for CO 2 and N 2 reduction journal January 2019
Recent progress in electrocatalytic nitrogen reduction journal January 2019
B 4 C nanosheets decorated with in situ -derived boron-doped graphene quantum dots for high-efficiency ambient N 2 fixation journal January 2019
Excavated cubic platinum–iridium alloy nanocrystals with high-index facets as highly efficient electrocatalysts in N 2 fixation to NH 3 journal January 2019
Boron and nitrogen dual-doped carbon nanospheres for efficient electrochemical reduction of N 2 to NH 3 journal January 2020
Electrochemical nitrogen fixation and utilization: theories, advanced catalyst materials and system design journal January 2019
MoP supported on reduced graphene oxide for high performance electrochemical nitrogen reduction journal January 2020
Promoting photocatalytic nitrogen fixation with alkali metal cations and plasmonic nanocrystals journal January 2019
Efficient electrocatalytic conversion of N 2 to NH 3 on NiWO 4 under ambient conditions journal January 2020
Pt-embedded in monolayer g-C 3 N 4 as a promising single-atom electrocatalyst for ammonia synthesis journal January 2019
Ambient dinitrogen electrocatalytic reduction for ammonia synthesis journal January 2019
Atomically dispersed metal dimer species with selective catalytic activity for nitrogen electrochemical reduction journal January 2019
Electrochemical reduction of N 2 to ammonia on Co single atom embedded N-doped porous carbon under ambient conditions journal January 2019
Aqueous electrocatalytic N 2 reduction for ambient NH 3 synthesis: recent advances in catalyst development and performance improvement journal January 2020
Ammonia Synthesis Under Ambient Conditions: Selective Electroreduction of Dinitrogen to Ammonia on Black Phosphorus Nanosheets journal January 2019
Electrochemical Synthesis of Ammonia: Recent Efforts and Future Outlook journal August 2019

Figures / Tables (4)

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75 CONDENSED MATTER PHYSICS
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