Directing the Surface Atomic Geometry on Copper Sulfide for Enhanced Electrochemical Nitrogen Reduction

Haneul Jin, Hee Soo Kim, Chi Ho Lee, Yongju Hong, Jihyun Choi, Hionsuck Baik, Sang Uck Lee, Sung Jong Yoo, Kwangyeol Lee, Hyun S. Park

Research output: Contribution to journalArticlepeer-review

7 Citations (Scopus)


Understanding catalytic-conversion determinants will blueprint an efficient electrocatalyst design for electrochemical nitrogen reduction. In metal chalcogenide-based catalysts, metal-site nitrogen adsorption initiates nitrogen fixation, and successive hydrogen supply from nearby chalcogen sites hydrogenates the nitrogen to ammonia. However, surface geometry-dependent reaction kinetics are rarely studied because the reaction is very fast. Here, we investigate the relationship between catalyst geometrical features and their electrochemical nitrogen reduction kinetics using surface atomic geometry-regulated copper sulfide (Cu1.81S) nanocatalysts with exposed (100)- and (010)-type facets for flat and zigzag planes, respectively. The exposed facet densities of the nanocatalysts are varied via their aspect ratios. Nanocrystals with highly exposed (010)-type surfaces exhibit the best nitrogen reduction kinetics. Density functional theory calculation reveals that the protruded Cu and S atomic arrangement on the zigzag (010)-type surface promotes N2adsorption and facilitates proton transfer from near the S site to*N2at the Cu site, thus fast-forwarding electrochemical nitrogen reduction.

Original languageEnglish
Pages (from-to)13638-13648
Number of pages11
JournalACS Catalysis
Issue number21
Publication statusPublished - 2022 Nov 4

Bibliographical note

Funding Information:
This work was supported by the National Research Foundation of Korea (NRF-2022M3I3A1094160, NRF-2021M3D1A2051389 (Creative Materials Discovery Program), NRF-2019R1A6A1A11044070, NRF-2020R1A2B5B03002475, NRF-2018M1A2A2061975, NRF-2021M3H4A1A02042948, NRF-2018M3D1A1058714, NRF-2021R1A2B5B01002879, and NRF-2022R1C1C2005786). This work was also supported by the Korea Institute of Science and Technology (2E31871). Y.H. acknowledges the Global Ph.D. Fellowship (NRF-2018H1A2A1062618).

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.


  • ammonia production
  • catalytic conversion
  • electrochemical nitrogen reduction
  • metal chalcogenide-based catalyst
  • surface atomic geometry

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry


Dive into the research topics of 'Directing the Surface Atomic Geometry on Copper Sulfide for Enhanced Electrochemical Nitrogen Reduction'. Together they form a unique fingerprint.

Cite this