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Photoelectrocatalytic hydrogen evolution and synchronous degradation of organic pollutants by pg-C_(3)N_(4)/β-FeOOH S-scheme heterojunction

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Science China(Technological Sciences) 2024年第4期67卷 1238-1252页

作者： LI XiBao HAN Tao ZHOU YingTang XIE Yu LUO YiDan HUANG JunTong CHEN Zhi DENG Fang School of Materials Science and engineering Nanchang Hangkong UniversityNanchang 330063China national-local joint engineering research center of heavy Metal pollutants control and resource utilization Nanchang Hangkong UniversityNanchang 330063China Zhejiang Key Laboratory of Petrochemical Environmental Pollution control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316022China

Crafting photoelectrocatalytic materials with robust oxidation-reduction properties for simultaneous hydrogen evolution and pollutant degradation poses a formidable challenge.In this study,a pg-C_(3)N_(4)/β-FeOOH S-scheme heterostructure with a special energy band structure was developed by anchoring porous pg-C_(3)N_(4)on needle shapedβ-FeOOH.Functioning as a hole extraction layer,needle-leaf-likeβ-FeOOH can facilitate efficient hole migration and enhance charge transport.Remarkably,the optimized 0.2-pg-C_(3)N_(4)/β-FeOOH could degrade 78%of ofloxacin(OFLO)in 90 min.The organic pollutants could absorb a large number of holes,which prompted a greater proportion of photogenerated electrons to actively participate in the hydrogen evolution reaction at the cathode.Consequently,the hydrogen production of 0.2-pg-C_(3)N_(4)/β-FeOOH reached 1452.88μmol cm^(-2)h^(-1),exhibiting a notable increase of 61.81-165.12μmol cm^(-2)h^(-1)compared with that in the absence of pollutants.Experimental and theoretical calculation results underscore that this investigation is grounded in a distinctive electron and hole dual channel transfer mechanism.These findings offer novel insights for the future development of S-scheme heterojunction photoelectrocatalytic materials capable of concurrently degrading pollutants and promoting hydrogen evolution.

关键词： photoelectrocatalysis hydrogen evolution degradation synchronous S-scheme heterojunction

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Rapid Degrading Carbamazepine in a Novel Advanced Oxidation Process of Bisulfite Activated by Lithium Cobaltate Recovered from Spent Lithium-ion Battery

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Chemical research in Chinese Universities 2024年第1期40卷 127-135页

作者： Yan Jiali Yang Kaiying Wang Xi Zhai Jinli Zhu Wenjie Yang Daoli Luo Yongming Gao Xiaoya Faculty of Environmental Science and engineering Kunming University of Science and TechnologyKunming650500P.R.China Innovation Team for Volatile Organic Compounds pollutants control and resource utilization of Yunnan Province Kunming650500P.R.China Higher Educational Key Laboratory for Odorous Volatile Organic Compounds pollutants control of Yunnan Province Kunming650500P.R.China

Maximizing the sustainable recycling of spent lithium-ion batteries(LIBs)shows economic and environmental significance.This study recovered lithium cobaltate(LiCoO_(2),LCO)from spent LIBs cathode powder.The recovered LCO was then combined with NaHSO_(3)to remove refractory organic pollutants of carbamazepine(CBZ)in water.The degradation of CBZ reached 80.0%within 60 min,by 1O_(2),SO_(4),OH and O_(2)^(-)generated in the LCO/NaHSO_(3)reaction.The electron transfer between Co(III)and Co(II)was beneficial to the generation of free radicals.The LCO/NaHSO_(3)degraded CBZ effectively in both secondary outlet water and tap water.However,high concentrations of inorganic ions(Cl^(−),HCO_(3)^(-),HPO_(4)^(2-),SO_(2)−4,NO_(3)^(-))and natural organic matter(humic acid,HA)could inhibit the degradation of CBZ.After three cycles,the stability of the LCO/NaHSO_(3)system was demonstrated by the maintained high efficiency in the degradation of CBZ.The obtained data indicate that the LCO/NaHSO_(3)system holds great application potential in the field of advanced oxidation degradation of pollutants.

关键词： Spent lithium-ion battery Lithium cobaltate Carbamazepine NaHSO_(3) Advanced oxidation

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Review of preferentially selective lithium extraction from spent lithium batteries: Principle and performance

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Journal of Energy Chemistry 2023年第3期78卷 253-261,I0008页

作者： Zhe Gao Meiting Huang Liming Yang Yufa Feng Yuan Ding Penghui Shao Xubiao Luo national-local joint engineering research center of heavy metals pollutants control and resource utilization Nanchang Hangkong UniversityNanchang 330063JiangxiChina

Lithium,as the lightest and lowest potential metal,is an ideal "battery metal" and the core strategic metal of the new energy industry revolution.Recovering lithium from spent lithium batteries(LIBs)has become one of the significant approaches to obtaining lithium resources.At present,the lithium extraction being generally placed at the last step of the spent LIBs recovery process has puzzles such as high acid consumption,low Li recovery purity and low recovery efficiency.Selective lithium extraction at the first step of the recovery process can effectively solve those puzzles.Since lithium leaching is a non-spontaneous reaction requiring additional energy to achieve,it is found that these methods can be divided into five ways according to the different types of energy driving the reaction occurring:(ⅰ)electric energy driving lithium extraction;(ⅱ) chemical energy driving lithium extraction;(ⅲ) mechanical energy driving lithium extraction;(ⅳ) thermal energy driving lithium extraction;(ⅴ) other energy driving lithium extraction.Through the analysis of the principle,reaction process and results of recovering lithium methods can provide a few directions for scholars’ subsequent research.It is necessary to speed up the exploration of the principle of these methods.It is expected that this study could provide a reference for the research on the selective lithium extraction.

关键词： Lithium Spent lithium batteries(LIBs) Recovery efﬁciency Preferentially Selective

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Lattice expansion boosting photocatalytic degradation performance of CuCo_(2)S_(4) with an inherent dipole moment

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Chinese Chemical Letters 2023年第2期34卷 355-361页

作者： Yicheng Guo Biguo Yan Fang Deng Penghui Shao Jianping Zou Xubiao Luo Shuqu Zhang Xibao Li national-local joint engineering research center of heavy Metal pollutants control and resource utilization Nanchang Hangkong UniversityNanchang 330063China

Realizing efficient charge separation and directional transfer is a challenge for single-component semiconductors.The spatial electric field generated by dipole moment could promote charge separation.Here,three-dimensional hierarchical Cu Co_(2)S_(4)microspheres with lattice distortion were prepared,and lattice distortion was modulated by changing feed Co/Cu molar ratios in synthesis.Cu Co_(2)S_(4)showed asymmetric crystal structure,leading to generation of dipole moment.The charge separation efficiency of Cu Co_(2)S_(4)was related to lattice distortion,and lattice expansion was in favor for charge separation.The Cu Co_(2)S_(4)with feed Cu/Co molar ratio of 1:4 (CCS-4) showed the maximum lattice expansion and exhibited the highest photocatalytic activity,which was attributable to the highest charge separation efficiency and the largest specific surface area.CCS-4 can remove 95.4%of tetracycline hydrochloride within 40 min photocatalysis,and effectively improve the biodegradability of pharmaceutical wastewater.Importantly,this study provides a new vision for constructing single-component photocatalysts with high photocatalytic performance.

关键词： CuCo_(2)S_(4) Lattice distortion Visible-light photocatalysis Structure-activity relationship Biodegradability improvement

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A pyrazine based metal-organic framework for selective removal of copper from strongly acidic solutions

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Frontiers of Environmental Science & engineering 2023年第3期17卷 75-86页

作者： Jiachuang Shao Penghui Shao Mingming Peng Min Li Ziwei Yao Xiuqin Xiong Caiting Qiu Yufan Zheng Liming Yang Xubiao Luo Key Laboratory of Jiangxi Province for Persistent pollutants control and resources Recycle National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource utilizationNanchang Hangkong UniversityNanchang 330063China Department of Chemical engineering Chongqing University of Science and TechnologyChongqing 401331China

The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection.Metal organic frameworks(MOFs)have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics,including adjustable structure,strong stability and porosity.Herein,pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic conditions.Selective copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic frameworks.Furthermore,the material exhibits excellent adsorption capacity,with a theoretical maximum copper uptake of 247 mg/g.As proven by XPS and FT-IR analysis,the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by pz-UiO-66.This work provides an opportunity for efficient and selective copper removal under strongly acidic conditions,and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.

关键词： Pyrazine Metal-organic frameworks Copper removal Strong acidity High selectivity

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Fabrication of supported acid catalytic composite fibers by a simple and low-cost method and their application on the synthesis of liquid biofuel 5-ethoxymethylfurfural

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Green Energy & Environment 2022年第1期7卷 165-171页

作者： Yinhua Yan Huiqin Guo Kexin Li Liushui Yan Key Laboratory of Jiangxi Province for Persistent pollutants control and resources Recycle NanChang Hangkong UniversityNanChang330063China national-local joint engineering research center of heavy metals Polluants control and resource utilization NanChang Hangkong UniversityNanChang330063China

In this paper,sulfonic groups functionalized annealed bio-based carbon microspheres loaded polytetrafluoroethylene(A-BCMSs-SO_(3)H@PTFE)fibers with high activity,high stability,and easy regeneration were successfully fabricated by a simple method using low-cost raw materials.The characterization results showed that the annealed biomass carbon microspheres derived from waste Camellia oleifera shells were evenly distributed on the polytetrafluoroethylene fibers and the sulfonic groups can be successfully loaded on the surface of annealed biomass carbon microspheres by room temperature sulfonation.Subsequently,the as-prepared A-BCMSs-SO_(3)H@PTFE fibers were applied to the acidcatalyzed synthesis of liquid biofuel 5-ethoxymethylfurfural.The catalytic experiment results indicated that the annealing temperature and time during catalyst preparation have a significant effect on the activity and selectivity of A-BCMSs-SO_(3)H@PTFE fibers.The results of catalytic reaction kinetics showed that the yield of 5-ethoxymethylfurfural can reach more than 60%after 72 h of acid-catalyzed reaction.The stability test showed that the as-prepared A-BCMSs-SO_(3)H@PTFE fibers still maintained a stable acid catalytic activity after four recycles.

关键词： Acid catalysis Waste Camellia oleifera shells Sulfonic groups Polytetrafluoroethylene fibers 5-Ethoxymethylfurfural

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Feasible fabrication of o-phenanthroline-based polymer adsorbent for selective capture of aqueous Ag(Ⅰ)

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Chinese Chemical Letters 2023年第3期34卷 191-194页

作者： Xuan Ding Wanjun Yu Xin Sheng Hui Shi Deng You Mingming Peng Penghui Shao Liming Yang Lingling Liu Xubiao Luo Key Laboratory of Jiangxi Province for Persistent pollutants control and resources Recycle Nanchang Hangkong UniversityNanchang 330063China national-local joint engineering research center of heavy metals pollutants control and resource utilization Nanchang Hangkong UniversityNanchang 330063China

Devising a desirable adsorbent for efficiently selective capture of Ag(Ⅰ) from wastewater has attracted much attention but faced with huge challenges. Herein, a novel linear o-phenanthroline-based polymer L-PRL was prepared via chemical oxidative polymerization for the adsorption of Ag(Ⅰ). The maximum adsorption capacity for Ag(Ⅰ) by L-PRL is 325.8 mg/g at pH 0. In addition, L-PRL owes ascendant selectivity for Ag(Ⅰ) from aqueous solutions containing various interfering metal ions of Pb(Ⅱ), Co(Ⅱ), Ni(Ⅱ), Cd(Ⅱ)and Fe(Ⅲ). Multiple characterizations of FT-IR and XPS uncover that the N groups on L-PRL act as adsorption sites to coordinate with Ag(Ⅰ). Density functional theory(DFT) calculations further evidence the mechanism that L-PRL is provided with the admirable adsorptivity and selectivity for Ag(Ⅰ). It is mainly attributed to the most stable complexes of L-PRL with Ag(Ⅰ), which possesses shortest Ag-N bond length compared with other heavy metal ions. Furthermore, 93.5% of initial adsorption capacity is reserved after four continuous regeneration cycles, indicating that L-PRL is equipped with superior recyclability and durability, and L-PRL is capable of removing Ag(Ⅰ) in low-concentration actual Ag(Ⅰ)-containing wastewater completely. This study shed light on the rational design of polymer adsorbents and in-depth insight into selective removal of aqueous Ag(Ⅰ).

关键词： Wastewater o-Phenanthroline Polymer Adsorbent Ag(Ⅰ) Selective capture

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Two-dimensional RGO-bridge S-scheme phosphorus-doped g-C_(3)N_(4)/Bi_(5)O_(7)Ivan der Waals heterojunctions for efficient visible-light photocatalytic treatment of real pharmaceutical wastewater

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中国科学:技术科学英文版 2023年第10期66卷 3011-3024页

作者： WANG ZhenZhou XU XiWei DENG Fang DIONYSIOU Dionysios D LI XiBao PENG JunLong LUO XuBiao ZOU JianPing LUO ShengLian national-local joint engineering research center of heavy Metal pollutants control and resource utilization Nanchang Hangkong UniversityNanchang 330063China Environmental engineering and Science Program Department of Chemical and Environmental Engineering(DChEE)University of CincinnatiCincinnati 45221-0012USA

The design of van der Waals heterojunctions with S-scheme charge transfer pathway is expected to be an effective strategy for improvement of photocatalytic performance.Herein,two-dimensional(2D)phosphorus-doped g-C_(3)N_(4)/Bi_(5)O_(7)Ivan der Waals heterojunctions with reduced graphene oxide as electron bridge(PCN/RGO/Bi_(5O)_(7)I)were successfully synthesized via hydrothermal method.The van der Waals interaction endowed 2D PCN/RGO/Bi_(5O)_(7)I with intimate contact interface,lattice match,tunable band structure,and internal electric field,which efficiently promoted interfacial charge separation and enhanced redox ability of photogenerated charge carriers.As a result,the S-scheme PCN/RGO/Bi_5O_7I van der Waals heterojunctions exhibited superior photocatalytic performance in ciprofloxacin degradation and real pharmaceutical wastewater treatment.The optimized 12%PCN/RGO/Bi_5O_7I displayed the highest photocatalytic activity with 92%removal of ciprofloxacin.Importantly,the COD removal efficiency and extent of mineralization of real pharmaceutical wastewater reached 66.9%and 59.8%,respectively,and the biodegradability of pharmaceutical wastewater was significantly improved.The photocatalytic mechanism of the S-scheme PCN/RGO/Bi_(5)O_(7)I van der Waals heterojunctions based on the analysis of reactive species,work function,and internal electric field was presented.This study provides fresh insights into plausible design of S-scheme van der Waals heterojunction to enhance photocatalytic redox ability.

关键词： S-scheme heterojunction van der Waals heterostructure photocatalytic degradation ciprofloxacin energy consumption

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One-step fabrication of mesoporous sulfur-doped carbon nitride for highly selective photocatalytic transformation of native lignin to monophenolic compounds

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Chinese Chemical Letters 2023年第1期34卷 440-445页

作者： Conghao Ku Huiqin Guo Kexin Li Qiong Wu Liushui Yan Key Laboratory of Jiangxi Province for Persistent pollutants control and resources Recycle Nanchang Hangkong UniversityNanchang 330063China national-local joint engineering research center of heavy metals pollutants control and resource utilization Nanchang Hangkong UniversityNanchang 330063China Jiangxi Provincial Experimental Teaching Demonstration center of Environmental Science and engineering Nanchang Hangkong UniversityNanchang 330063China

Photocatalytic selective transform native lignin into valuable chemicals is an attractive but challenging task.Herein,we report a mesoporous sulfur-doped carbon nitride(MSCN-0.5)which is prepared by a facile one-step thermal condensation strategy.It is highly active and selective for the cleavage Cα-Cβbond inβ-O-4 lignin model compound under visible light radiation at room temperature,achieving 99%substrate conversion and 98%Cα-Cβbond cleavage selectivity.Mechanistic studies revealed that the Cβ-H bond of lignin model compounds activated by holes and generate key Cβradical intermediates,further induced the Cα-Cβbond cleavage by superoxide anion radicals(·O2-)to produce aromatic oxygenates.Waste Camellia oleifera shell(WCOS)was taken as a representative to further understand the reaction mechanisms on native lignin.33.2 mg of monophenolic compounds(Vanillin accounted for 22%and Syringaldehyde for 34%)can be obtained by each gram of WCOS lignin,which is 2.5 times as that of the pristine carbon nitride.The present work offers useful guidance for designing metal-free heterogeneous photocatalysts for Cα-Cβbond cleavage to harvest monophenolic compounds.

关键词： Mesostructure Sulfur-doped carbon nitride Photocatalysis Lignin model compound Native lignin Monophenolic compounds

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Health risk assessment of heavy metal pollution in groundwater of a karst basin,SW China

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Journal of Groundwater Science and engineering 2024年第1期12卷 49-61页

作者： Fu-ning Lan Yi Zhao Jun Li Xiu-qun Zhu Karst Ecosystem National Observation and Research StationPingguo 531406GuangxiChina Institute of Karst Geology International Research Centre on KarstUnder the Auspices of UNESCOGuangxi Karst Resources and Environment Research Center of Engineering TechnologyChinese Academy of Geological SciencesKarst Dynamics LaboratoryMNR and GuangxiGuilin 541004China Hebei Key Laboratory of Water Quality engineering and Comprehensive utilization of Water resources Hebei University of ArchitectureZhangjiakou 075000Hebei ProvinceChina College of Hydrology and Water resources Hohai UniversityNanjing 210098China

To investigate the presence of metal elements and assess their health risk for the populace in the Nandong Underground River Basin(NURB),we conducted an analysis of eleven common heavy metals in the water body.A Health risk assessment(HRA)model was employed to analyze 84 water samples from the NURB.The detection results revealed the following order of heavy metals concentrations:Fe>Al>Mn>Zn>As>Cd>Pb>Cr>Ni>Cu>Hg.Correlation analysis indicated a certain similarity in material source and migration transformation among these eleven metal elements.Our study identified that the health risks for local residents exposed to metal elements in the water of NURB primarily stem from carcinogenic risk(10^(−6)–10^(−4)a^(−1))through the drinking water pathway.Moreover,the health risk of heavy metal exposure for children through drinking water was notably higher than for adults.The maximum health risks of Cr in both underground and surface water exceeded the recommendation standard(5.0×10^(−5)a^(−1))from ICRP,surpassing the values recommended by the Swedish Environmental Protection Agency,the Dutch Ministry of Construction and Environment and the British Royal Society(5.0×10^(−6)a^(−1)).The results of the health risk assessment indicate that Cr in the water of NURB is the primary source of carcinogenic risk for local residents,followed by Cd and As.Consequently,it is imperative to control these three carcinogenic metals when the water was used as drinking water resource.

关键词： Water Pollution Correlation Analysis Toxicity of heavy Metal Elements Underground River Basin Carcinogenicity Potential

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