Eggshell membrane derived nitrogen rich porous carbon for selective electrosorption of nitrate from water

Jiao Chen; Kuichang Zuo; Yilin Li; Xiaochuan Huang; Jiahui Hu; Ying Yang; Weipeng Wang; Long Chen; Amit Jain; Rafael Verduzco; Xiaoyan Li; Qilin Li

doi:10.1016/j.watres.2022.118351

Eggshell membrane derived nitrogen rich porous carbon for selective electrosorption of nitrate from water

Water Res. 2022 Jun 1:216:118351. doi: 10.1016/j.watres.2022.118351. Epub 2022 Mar 22.

Authors

Jiao Chen¹, Kuichang Zuo², Yilin Li³, Xiaochuan Huang⁴, Jiahui Hu⁵, Ying Yang⁶, Weipeng Wang⁷, Long Chen⁸, Amit Jain⁹, Rafael Verduzco⁹, Xiaoyan Li⁵, Qilin Li¹⁰

Affiliations

¹ Shenzhen Engineering Research Laboratory for Sludge and Food Waste Treatment and Resource Recovery, Tsinghua Shenzhen International Graduate School, Tsinghua University, China; Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston, Texas 77005, USA.
² Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston, Texas 77005, USA; The Key Laboratory of Water and Sediment Sciences, Ministry of Education; College of Environment Sciences and Engineering, Peking University, Beijing 100871, China; NSF Nanosystems Engineering Research Center Nanotechnology-Enabled Water Treatment, Rice University, MS 6398, 6100 Main Street, Houston, Texas 77005, USA. Electronic address: kuichang.zuo@pku.edu.cn.
³ Department of Chemical and Biomolecular Engineering, Rice University, MS 362, 6100 Main Street, Houston, Texas 77005, USA.
⁴ Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston, Texas 77005, USA; The Key Laboratory of Water and Sediment Sciences, Ministry of Education; College of Environment Sciences and Engineering, Peking University, Beijing 100871, China.
⁵ Shenzhen Engineering Research Laboratory for Sludge and Food Waste Treatment and Resource Recovery, Tsinghua Shenzhen International Graduate School, Tsinghua University, China.
⁶ Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston, Texas 77005, USA.
⁷ Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston, Texas 77005, USA; Department of Materials Science and Nano Engineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
⁸ Department of Materials Science and Nano Engineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA.
⁹ Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston, Texas 77005, USA; Department of Chemical and Biomolecular Engineering, Rice University, MS 362, 6100 Main Street, Houston, Texas 77005, USA.
¹⁰ Civil and Environmental Engineering, Rice University, MS 319, 6100 Main Street, Houston, Texas 77005, USA; The Key Laboratory of Water and Sediment Sciences, Ministry of Education; College of Environment Sciences and Engineering, Peking University, Beijing 100871, China; NSF Nanosystems Engineering Research Center Nanotechnology-Enabled Water Treatment, Rice University, MS 6398, 6100 Main Street, Houston, Texas 77005, USA; Department of Chemical and Biomolecular Engineering, Rice University, MS 362, 6100 Main Street, Houston, Texas 77005, USA; Department of Materials Science and Nano Engineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA. Electronic address: qilin.li@rice.edu.

PMID: 35390703
DOI: 10.1016/j.watres.2022.118351

Abstract

Nitrate (NO₃^-) is a ubiquitous contaminant in water and wastewater. Conventional treatment processes such as adsorption and membrane separation suffer from low selectivity for NO₃^- removal, causing high energy consumption and adsorbents usage. In this study, we demonstrate selective removal of NO₃^- in an electrosorption process by a thin, porous carbonized eggshell membrane (CESM) derived from eggshell bio-waste. The CESM possesses an interconnected hierarchical pore structure with pore size ranging from a few nanometers to tens of micrometers. When utilized as the anode in an electrosorption process, the CESM exhibited strong selectivity for NO₃^- over Cl^-, SO₄^2-, and H₂PO₄^-. Adsorption of NO₃^- by the CESM reached 2.4 × 10^-3 mmol/m², almost two orders of magnitude higher than that by activated carbon (AC). More importantly, the CESM achieved NO₃^-/Cl^- selectivity of 7.79 at an applied voltage of 1.2 V, the highest NO₃^-/Cl^- selectivity reported to date. The high selectivity led to a five-fold reduction in energy consumption for NO₃^- removal compared to electrosorption using conventional AC electrodes. Density function theory calculation suggests that the high NO₃^- selectivity of CESM is attributed to its rich nitrogen-containing functional groups, which possess higher binding energy with NO₃^- compared to Cl^-, SO₄^2-, and H₂PO₄^-. These results suggest that nitrogen-rich biomaterials are good precursors for NO₃^- selective electrodes; similar chemistry can also be used in other materials to achieve NO₃^- selectivity.

Keywords: Density functional theory; Eggshell membrane; Electrosorption; Nitrate selectivity; Nitrogen functional groups.

MeSH terms

Animals
Charcoal
Egg Shell
Electrodes
Nitrates* / chemistry
Nitrogen
Nitrogen Oxides
Porosity
Wastewater
Water
Water Purification* / methods

Substances

Nitrates
Nitrogen Oxides
Waste Water
Water
Charcoal
Nitrogen