Enhancement of NH3Production in Electrochemical N2Reduction by the Cu-Rich Inner Surfaces of Beveled CuAu Nanoboxes

Biva Talukdar, Tung Chun Kuo, Brian T. Sneed, Lian Ming Lyu, Hung Min Lin, Yu Chun Chuang, Mu Jeng Cheng, Chun Hong Kuo

Research output: Contribution to journalReview articlepeer-review

Abstract

The global ammonia yield is critical to the fertilizer industry as the global food demand is highly dependent on it, whereas, NH3 is also a key chemical for pharmaceutical, textile, plastic, explosive, and dye-making industries. At present, the demand for NH3 is fulfilled by the Haber-Bosch method, which consumes 1-3% of global energy and causes 0.5-1% CO2 emission every year. To reduce emissions and improve energy efficiency, the electrochemical nitrogen gas reduction reaction (N2RR) has received much attention and support after the funding announcement by the U.S. Department of Energy. In this work, we have created hollow CuAu nanoboxes with Cu-rich inner walls to improve the NH3 Faradaic efficiency in N2RR. These beveled nanoboxes are produced in different degrees of corner and edge etching, which produces both polyhedral and concave structures. In N2RR, the binary CuAu nanoboxes enhanced NH3 production compared to individual Au and Cu nanocubes. The results of DFT calculations suggest the Cu-rich inner walls in the hollow beveled CuAu nanoboxes play a major role in their performance by reducing the free energy ΔG*NNH for the potential-determining step to form *NNH (∗ + N2(g) + H+ + e- → *NNH). Meanwhile, the results in 10-cycle and solar-illuminated N2RR indicate the beveled CuAu nanoboxes are not only robust electrocatalysts but show promise in photocatalysis as well.

Original languageEnglish
JournalACS Applied Materials and Interfaces
DOIs
Publication statusAccepted/In press - 2021

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

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