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Enhancing Hydrogen Diffusion in Catalytic Removal of Nitrate Using a Flow Reactor

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Abstract

The excessive application of nitrogen fertilizers, pesticides and sewage irrigation in agriculture has caused serious nitrate pollution in natural water systems. Selective catalytic reduction of nitrate (NO3−) with hydrogen (H2) to dinitrogen (N2) is a promising approach to address this public health risk, but the practical application of this denitrification technology is currently limited by the low NO3− removal rate and the high cost of palladium-based catalysts. In this work, we report an integrated thermo/electro-catalytic flow reactor for nitrate reduction. The innovative design of the solid–gas–liquid triple-phase interface enables high-throughput catalytic reduction of NO3− to N2. H2 can be either supplied to the flow cell from an external source or produced in situ via the integrated water electrolyzer unit. The H2 utilization efficiency of the reported flow reactor is increased significantly over what observed in conventional batch reactors. Moreover, a surface Pd enriched Cu@Pd catalyst was synthesized by galvanic replacement to boost Pd utilization. The Cu@Pd catalyst showed an unprecedented specific NO3− removal rate of \(\sim 15.5\;{\text{mM}}_{{{\text{NO}}_{3}^{ - } }} \;{\text{g}}_{{{\text{Pd}}^{ - 1} }} \;\min^{ - 1}\).

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Data Availability

The data that support the finding of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

The authors thank the Delaware Energy Institute for the financial support.

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Authors and Affiliations

  1. Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA

    Hongjie Tang, Emily Jeng, Yushan Yan, Bingjun Xu & Feng Jiao

  2. Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 610054, Chengdu, Sichuan, China

    Yijin Kang

  3. College of Chemistry and Molecular Engineering, Peking University, 100871, Beijing, China

    Bingjun Xu

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  1. Hongjie Tang
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  2. Emily Jeng
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  3. Yijin Kang
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  4. Yushan Yan
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  6. Feng Jiao
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Correspondence to Yushan Yan, Bingjun Xu or Feng Jiao.

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Tang, H., Jeng, E., Kang, Y. et al. Enhancing Hydrogen Diffusion in Catalytic Removal of Nitrate Using a Flow Reactor. Top Catal 66, 1260–1269 (2023). https://doi.org/10.1007/s11244-023-01837-0

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