Xue-Qi Fan , Yi-Man Sun , Le Tao , Shu-Xia Guan , De-Bin Ji
{"title":"双氮源锚定生物炭通过吸附-还原耦合机制实现了对废水中Cr(VI)的高效去除","authors":"Xue-Qi Fan , Yi-Man Sun , Le Tao , Shu-Xia Guan , De-Bin Ji","doi":"10.1016/j.jece.2025.119237","DOIUrl":null,"url":null,"abstract":"<div><div>In this study, a dual-nitrogen-source modified biochar material (N<sub>400</sub>-BC/P<sub>10</sub>) was developed via an ultrasonic-assisted hydrothermal method for the efficient removal of hexavalent chromium (Cr(VI)). Skeleton nitrogen structures such as pyridinic nitrogen and pyrrolic nitrogen were introduced through urea doping, while amino groups were grafted on the surface using polyethyleneimine (PEI). This modification strategy achieved the synergistic enhancement of “skeleton nitrogen” and “functional group nitrogen”. N<sub>400</sub>-BC/P<sub>10</sub> exhibited a high affinity toward Cr(VI). At pH 2, the adsorption capacity of the material progressively increased with the augmentation of nitrogen content. At an initial concentration of 200 mg·L<sup>−1</sup>, N<sub>400</sub>-BC/P<sub>10</sub> exhibited an order-of-magnitude increase for Cr(VI) equilibrium adsorption capacity (340.02 mg·g<sup>−1</sup>) compared with that of single-nitrogen-source modified counterpart (251.36 mg·g<sup>−1</sup>). Even in the presence of interfering coexisting anions and cations, N<sub>400</sub>-BC/P<sub>10</sub> maintained an adsorption capacity of at least 296.68 mg·g<sup>−1</sup> and a removal efficiency of at least 74 %. The adsorption process followed the pseudo-second-order kinetics and the Langmuir isotherm model, indicating that chemical adsorption was the predominant mechanism. XPS analysis revealed that the removal of Cr(VI) by N<sub>400</sub>-BC/P<sub>10</sub> followed a coupled mechanism of “adsorption-reduction-stabilization”. Moreover, N<sub>400</sub>-BC/P<sub>10</sub> demonstrated excellent practical wastewater treatment capability, highlighting its significant potential for industrial wastewater treatment. The dual-nitrogen-source anchoring strategy proposed in this study provides a new paradigm for the design of biochar-based heavy metal removal materials with high performance, low cost, and low environmental load. Furthermore, the detailed adsorption-reduction coupling mechanism also provides a theoretical basis for the precision remediation of heavy metal pollution.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":"13 6","pages":"Article 119237"},"PeriodicalIF":7.2000,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Dual-nitrogen-source anchored biochar achieves efficient removal of Cr(VI) from wastewater through an adsorption-reduction coupling mechanism\",\"authors\":\"Xue-Qi Fan , Yi-Man Sun , Le Tao , Shu-Xia Guan , De-Bin Ji\",\"doi\":\"10.1016/j.jece.2025.119237\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this study, a dual-nitrogen-source modified biochar material (N<sub>400</sub>-BC/P<sub>10</sub>) was developed via an ultrasonic-assisted hydrothermal method for the efficient removal of hexavalent chromium (Cr(VI)). Skeleton nitrogen structures such as pyridinic nitrogen and pyrrolic nitrogen were introduced through urea doping, while amino groups were grafted on the surface using polyethyleneimine (PEI). This modification strategy achieved the synergistic enhancement of “skeleton nitrogen” and “functional group nitrogen”. N<sub>400</sub>-BC/P<sub>10</sub> exhibited a high affinity toward Cr(VI). At pH 2, the adsorption capacity of the material progressively increased with the augmentation of nitrogen content. At an initial concentration of 200 mg·L<sup>−1</sup>, N<sub>400</sub>-BC/P<sub>10</sub> exhibited an order-of-magnitude increase for Cr(VI) equilibrium adsorption capacity (340.02 mg·g<sup>−1</sup>) compared with that of single-nitrogen-source modified counterpart (251.36 mg·g<sup>−1</sup>). Even in the presence of interfering coexisting anions and cations, N<sub>400</sub>-BC/P<sub>10</sub> maintained an adsorption capacity of at least 296.68 mg·g<sup>−1</sup> and a removal efficiency of at least 74 %. The adsorption process followed the pseudo-second-order kinetics and the Langmuir isotherm model, indicating that chemical adsorption was the predominant mechanism. XPS analysis revealed that the removal of Cr(VI) by N<sub>400</sub>-BC/P<sub>10</sub> followed a coupled mechanism of “adsorption-reduction-stabilization”. Moreover, N<sub>400</sub>-BC/P<sub>10</sub> demonstrated excellent practical wastewater treatment capability, highlighting its significant potential for industrial wastewater treatment. The dual-nitrogen-source anchoring strategy proposed in this study provides a new paradigm for the design of biochar-based heavy metal removal materials with high performance, low cost, and low environmental load. Furthermore, the detailed adsorption-reduction coupling mechanism also provides a theoretical basis for the precision remediation of heavy metal pollution.</div></div>\",\"PeriodicalId\":15759,\"journal\":{\"name\":\"Journal of Environmental Chemical Engineering\",\"volume\":\"13 6\",\"pages\":\"Article 119237\"},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2025-09-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2213343725039338\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343725039338","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Dual-nitrogen-source anchored biochar achieves efficient removal of Cr(VI) from wastewater through an adsorption-reduction coupling mechanism
In this study, a dual-nitrogen-source modified biochar material (N400-BC/P10) was developed via an ultrasonic-assisted hydrothermal method for the efficient removal of hexavalent chromium (Cr(VI)). Skeleton nitrogen structures such as pyridinic nitrogen and pyrrolic nitrogen were introduced through urea doping, while amino groups were grafted on the surface using polyethyleneimine (PEI). This modification strategy achieved the synergistic enhancement of “skeleton nitrogen” and “functional group nitrogen”. N400-BC/P10 exhibited a high affinity toward Cr(VI). At pH 2, the adsorption capacity of the material progressively increased with the augmentation of nitrogen content. At an initial concentration of 200 mg·L−1, N400-BC/P10 exhibited an order-of-magnitude increase for Cr(VI) equilibrium adsorption capacity (340.02 mg·g−1) compared with that of single-nitrogen-source modified counterpart (251.36 mg·g−1). Even in the presence of interfering coexisting anions and cations, N400-BC/P10 maintained an adsorption capacity of at least 296.68 mg·g−1 and a removal efficiency of at least 74 %. The adsorption process followed the pseudo-second-order kinetics and the Langmuir isotherm model, indicating that chemical adsorption was the predominant mechanism. XPS analysis revealed that the removal of Cr(VI) by N400-BC/P10 followed a coupled mechanism of “adsorption-reduction-stabilization”. Moreover, N400-BC/P10 demonstrated excellent practical wastewater treatment capability, highlighting its significant potential for industrial wastewater treatment. The dual-nitrogen-source anchoring strategy proposed in this study provides a new paradigm for the design of biochar-based heavy metal removal materials with high performance, low cost, and low environmental load. Furthermore, the detailed adsorption-reduction coupling mechanism also provides a theoretical basis for the precision remediation of heavy metal pollution.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.