Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron Extraction

Abstract Green and eco‐friendly iron‐based materials for efficient Cr(VI) removal have attracted considerable interest, but challenges related to narrow working pH ranges and iron utilization efficiency still remain. Herein, inspired by the hot‐spot effect‐triggered confined coordination strategy, a...

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Main Authors: Yue Wang, Hongyu Li, Hao Liu, Chengsi Hou, Zhengwei Zhou, Shuai Peng, Zuofeng Chen, Zhendong Lei, Deli Wu
Format: Article
Language:English
Published: Wiley 2025-04-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202417368
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author Yue Wang
Hongyu Li
Hao Liu
Chengsi Hou
Zhengwei Zhou
Shuai Peng
Zuofeng Chen
Zhendong Lei
Deli Wu
author_facet Yue Wang
Hongyu Li
Hao Liu
Chengsi Hou
Zhengwei Zhou
Shuai Peng
Zuofeng Chen
Zhendong Lei
Deli Wu
author_sort Yue Wang
collection DOAJ
description Abstract Green and eco‐friendly iron‐based materials for efficient Cr(VI) removal have attracted considerable interest, but challenges related to narrow working pH ranges and iron utilization efficiency still remain. Herein, inspired by the hot‐spot effect‐triggered confined coordination strategy, a biomass‐confined iron‐based reductant (CMC‐GTB/Febm) is designed for Cr(VI) reduction and detoxification. Electron enrichment and confinement on biomass carriers are achieved through electron transfer mediated by coordination interactions between anchored iron species and biomass. Thus, the CMC‐GTB/Febm achieved 99% Cr(VI) reduction at circumneutral pH (5–9), with a maximum removal capacity of 180 mg g−1. Under iron dosing close to the stoichiometric ratio (Fe/Cr = 3/1), the Cr(VI) removal kinetics and efficiency of CMC‐GTB/Febm are 53.2–870.5 and 5.5–48.8 times higher than those of micro‐ or nano‐zero‐valent iron (ZVI), respectively. Mechanistic analyses revealed that confined electron transfer is facilitated by coordination interactions between biomass and anchored iron species, which enhanced Cr(VI) reduction. Moreover, biomass‐tethered reduced Cr(III) is stabilized by electrostatic adsorption and biomass‐Cr(III) coordination, which ultimately detoxifies the phytotoxicity of Cr(VI). The conversion of this strategy to kilogram‐scale production and the simulated Cr(VI) removal in real water matrices are confirmed. This study provides a basis for the controlled design and industrial application of environmentally friendly iron‐based reductants.
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spelling doaj-art-f562117c7e4e4e23abff242d27f6704c2025-08-20T03:18:06ZengWileyAdvanced Science2198-38442025-04-011215n/an/a10.1002/advs.202417368Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron ExtractionYue Wang0Hongyu Li1Hao Liu2Chengsi Hou3Zhengwei Zhou4Shuai Peng5Zuofeng Chen6Zhendong Lei7Deli Wu8State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaState Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaState Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaState Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaState Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaState Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaSchool of Chemical Science and Engineering Tongji University Shanghai 200092 P. R. ChinaState Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaState Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. ChinaAbstract Green and eco‐friendly iron‐based materials for efficient Cr(VI) removal have attracted considerable interest, but challenges related to narrow working pH ranges and iron utilization efficiency still remain. Herein, inspired by the hot‐spot effect‐triggered confined coordination strategy, a biomass‐confined iron‐based reductant (CMC‐GTB/Febm) is designed for Cr(VI) reduction and detoxification. Electron enrichment and confinement on biomass carriers are achieved through electron transfer mediated by coordination interactions between anchored iron species and biomass. Thus, the CMC‐GTB/Febm achieved 99% Cr(VI) reduction at circumneutral pH (5–9), with a maximum removal capacity of 180 mg g−1. Under iron dosing close to the stoichiometric ratio (Fe/Cr = 3/1), the Cr(VI) removal kinetics and efficiency of CMC‐GTB/Febm are 53.2–870.5 and 5.5–48.8 times higher than those of micro‐ or nano‐zero‐valent iron (ZVI), respectively. Mechanistic analyses revealed that confined electron transfer is facilitated by coordination interactions between biomass and anchored iron species, which enhanced Cr(VI) reduction. Moreover, biomass‐tethered reduced Cr(III) is stabilized by electrostatic adsorption and biomass‐Cr(III) coordination, which ultimately detoxifies the phytotoxicity of Cr(VI). The conversion of this strategy to kilogram‐scale production and the simulated Cr(VI) removal in real water matrices are confirmed. This study provides a basis for the controlled design and industrial application of environmentally friendly iron‐based reductants.https://doi.org/10.1002/advs.202417368circumneutral pHconfined coordination reactionCr(VI) detoxification and tetheringgreen synthesisscale‐up extended application
spellingShingle Yue Wang
Hongyu Li
Hao Liu
Chengsi Hou
Zhengwei Zhou
Shuai Peng
Zuofeng Chen
Zhendong Lei
Deli Wu
Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron Extraction
Advanced Science
circumneutral pH
confined coordination reaction
Cr(VI) detoxification and tethering
green synthesis
scale‐up extended application
title Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron Extraction
title_full Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron Extraction
title_fullStr Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron Extraction
title_full_unstemmed Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron Extraction
title_short Mechanochemical‐Triggered Confined Coordination of Iron‐Biomass Composites for Efficient Cr(VI) Reduction Under Circumneutral pH Via Accelerated Electron Extraction
title_sort mechanochemical triggered confined coordination of iron biomass composites for efficient cr vi reduction under circumneutral ph via accelerated electron extraction
topic circumneutral pH
confined coordination reaction
Cr(VI) detoxification and tethering
green synthesis
scale‐up extended application
url https://doi.org/10.1002/advs.202417368
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