Self-Standing Porous Aromatic Framework Electrodes for Efficient Electrochemical Uranium Extraction DOI Creative Commons

Dingyang Chen,

Yue Li,

Xinyue Zhao

et al.

ACS Central Science, Journal Year: 2023, Volume and Issue: 9(12), P. 2326 - 2332

Published: Dec. 13, 2023

Electrochemical uranium extraction from seawater provides a new opportunity for sustainable supply of nuclear fuel. However, there is still room studying flexible electrode materials in this field. Herein, we construct amidoxime group modified porous aromatic frameworks (PAF-144-AO) on carbon cloths situ using an easy to scale-up electropolymerization method followed by postdecoration fabricate the self-standing, binder-free, metal-free electrodes (PAF-E). Based architectural design, adsorption sites (amidoxime groups) and catalytic (carbazole are integrated into PAF-144-AO. Under action alternating electric field, uranyl ions selectively captured PAN-E subsequently transformed Na2O(UO3·H2O)x precipitates presence Na+ via reversible electron transfer, with capacity 12.6 mg g–1 over 24 days natural seawater. This adsorption–electrocatalysis mechanism also demonstrated at molecular level ex spectroscopy. Our work offers effective approach designing organic polymer electrodes, which hold great potential field electrochemical

Language: Английский

Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance DOI Creative Commons
Zhongshan Chen, Jingyi Wang, Mengjie Hao

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Feb. 27, 2023

Covalent organic frameworks (COFs) represent an emerging class of photocatalysts. However, their complicated structures lead to indeterminacy about photocatalytic active sites and reaction mechanisms. Herein, we use reticular chemistry construct a family isoreticular crystalline hydrazide-based COF photocatalysts, with the optoelectronic properties local pore characteristics COFs modulated using different linkers. The excited state electronic distribution transport pathways in are probed host experimental methods theoretical calculations at molecular level. One our developed (denoted as COF-4) exhibits remarkable electron utilization efficiency charge transfer properties, achieving record-high uranium extraction performance ~6.84 mg/g/day natural seawater among all techniques reported so far. This study brings new understanding operation COF-based guiding design improved photocatalysts for many applications.

Language: Английский

Citations

283

Functionalized Iron–Nitrogen–Carbon Electrocatalyst Provides a Reversible Electron Transfer Platform for Efficient Uranium Extraction from Seawater DOI
Hui Yang, Xiaolu Liu, Mengjie Hao

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(51)

Published: Oct. 4, 2021

Uranium extraction from seawater provides an opportunity for sustainable fuel supply to nuclear power plants. Herein, adsorption-electrocatalysis strategy is demonstrated efficient uranium using a functionalized iron-nitrogen-carbon (Fe-Nx -C-R) catalyst, comprising N-doped carbon capsules supporting FeNx single-atom sites and surface chelating amidoxime groups (R). The bring hydrophilicity the adsorbent offer surface-specific binding UO22+ capture. site-isolated centres reduce adsorbed UO2+ . Subsequently, through electrochemical reduction of sites, unstable U(V) ions are reoxidized U(VI) in presence Na+ resulting generation solid Na2 O(UO3 ·H2 O)x , which can easily be collected. Fe-Nx -C-R reduced concentration ≈3.5 ppb below 0.5 with calculated capacity ≈1.2 mg g-1 within 24 h. To best knowledge, developed system first use adsorption uranyl electrodeposition .H2 seawater. important discoveries guide technology development

Language: Английский

Citations

277

Tuning Local Charge Distribution in Multicomponent Covalent Organic Frameworks for Dramatically Enhanced Photocatalytic Uranium Extraction DOI
Hui Yang, Mengjie Hao,

Yinghui Xie

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: April 29, 2023

Optimizing the electronic structure of covalent organic framework (COF) photocatalysts is essential for maximizing photocatalytic activity. Herein, we report an isoreticular family multivariate COFs containing chromenoquinoline rings in COF and electron-donating or withdrawing groups pores. Intramolecular donor-acceptor (D-A) interactions allowed tuning local charge distributions carrier separation under visible light irradiation, resulting enhanced performance. By optimizing optoelectronic properties COFs, a uranium extraction efficiency 8.02 mg/g/day was achieved using nitro-functionalized multicomponent natural seawater, exceeding performance all reported to date. Results demonstrate effective design strategy towards high-activity with intramolecular D-A structures not easily accessible traditional synthetic approaches.

Language: Английский

Citations

195

Highly Efficient Electrocatalytic Uranium Extraction from Seawater over an Amidoxime‐Functionalized In–N–C Catalyst DOI
Xiaolu Liu,

Yinghui Xie,

Mengjie Hao

et al.

Advanced Science, Journal Year: 2022, Volume and Issue: 9(23)

Published: June 17, 2022

Seawater contains uranium at a concentration of ≈3.3 ppb, thus representing rich and sustainable nuclear fuel source. Herein, an adsorption-electrocatalytic platform is developed for extraction from seawater, comprising atomically dispersed indium anchored on hollow nitrogen-doped carbon capsules functionalized with flexible amidoxime moieties (In-N

Language: Английский

Citations

185

Functional nanomaterials for selective uranium recovery from seawater: Material design, extraction properties and mechanisms DOI
You Wu,

Yinghui Xie,

Xiaolu Liu

et al.

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 483, P. 215097 - 215097

Published: March 6, 2023

Language: Английский

Citations

156

Confining Ti-oxo clusters in covalent organic framework micropores for photocatalytic reduction of the dominant uranium species in seawater DOI Creative Commons
Shuo Zhang, Lixi Chen,

Zhiying Qu

et al.

Chem, Journal Year: 2023, Volume and Issue: 9(11), P. 3172 - 3184

Published: July 11, 2023

Language: Английский

Citations

95

Porous Materials for Water Purification DOI Creative Commons
Yanpei Song,

Joshua Phipps,

Changjia Zhu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(11)

Published: Dec. 20, 2022

Abstract Water pollution is a growing threat to humanity due the pervasiveness of contaminants in water bodies. Significant efforts have been made separate these hazardous components purify polluted through various methods. However, conventional remediation methods suffer from limitations such as low uptake capacity or selectivity, and current quality standards cannot be met. Recently, advanced porous materials (APMs) shown promise improved segregation compared traditional selectivity. These feature merits high surface area versatile functionality, rendering them ideal platforms for design novel adsorbents. This Review summarizes development employment APMs variety treatments accompanied by assessments task‐specific adsorption performance. Finally, we discuss our perspectives on future opportunities purification.

Language: Английский

Citations

88

Emerging technologies for uranium extraction from seawater DOI
Hui Yang, Yanfang Liu, Zhongshan Chen

et al.

Science China Chemistry, Journal Year: 2022, Volume and Issue: 65(12), P. 2335 - 2337

Published: Sept. 22, 2022

Language: Английский

Citations

76

Strategies for designing highly efficient adsorbents to capture uranium from seawater DOI
Yun Li, Ya‐Jun Zheng,

Zia Ahamd

et al.

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 491, P. 215234 - 215234

Published: May 26, 2023

Language: Английский

Citations

63

Recent progress of radionuclides separation by porous materials DOI

Yinghui Xie,

Long Yu, Long Chen

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(11), P. 3515 - 3577

Published: Sept. 26, 2024

Language: Английский

Citations

63