RESOURCES CONSERVATION AND RECYCLING
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2021
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IF 10.204
Liming Yang,Genping Yi,Bo Wang,Penghui Shao,Yufa Feng,Yanbiao Liu,Kai Yu,Fuqiang Liu,Lingling Liu,Xubiao Luo,Shenglian Luo
Simultaneous recovery and value-added conversion of hazardous heavy metal ions from complex wastewater sources is of great significance yet challenging. Herein, we demonstrate that highly toxic antimonite Sb(III) could be effectively recovered from antimony (Sb) mine flotation wastewater and converted into high-value-added metallic Sb using a novel facile atomic H* enhanced electrochemical reduction avenue coupled with thermal reduction by H 2 gas. The high production of atomic H* generated from the electrochemical cathode with an optimum reduction potential of –1.2 V vs . Ag/AgCl, which is lower than the Sb(III) reduction potential of –1.0 V, might be attributable to the superior Sb recovery capabilities. Furthermore, the metallic Sb concentration at –1.2 V was 14.43 times greater than at –1.0 V due to the strong reductivity of atomic H*. In addition, Sb(III) removal efficiency was found to be as high as 98.52%, with a metallic Sb recovery rate of up to 1.67 mg min –1 . The efficiency of Sb(III) recovery was demonstrated throughout a wide pH range, with metallic Sb being the main product, independent of the presence of multiple coexisting ions. Economic analysis also indicated that treating Sb mine flotation wastewater per ton may yield a net profit of $40.09. This research contributes to the advancement of an atomic H* enhanced electrochemical technology for high-valued heavy metal recovery from complex heavy metal-polluted wastewater.
研究领域:
环境科学
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冶金工程
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电化学工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Tian Liu,Jinming Luo,Xiaoyang Meng,Liming Yang,Bin Liang,Meijun Liu,Chengbin Liu,Aijie Wang,Xia Liu,Yong Pei,Jili Yuan,John Crittenden
Although noble metal electrocatalysts are highly efficient in the dehalogenation of halogenated antibiotics, the prohibitive cost hinders their practical applications. In this study, a cobalt-phosphorous/oxide (Co P/O) composite prepared via a one-step electrodeposition was for the first time applied in electroreductive dechlorination of halogenated antibiotics (HA), including chloramphenicol (CAP), florfenicol (FLO) and thiamphenicol (TAP). Co P/O had a higher FLO dechlorination efficiency (91%) than Pd/C (69.3%) (t = 60 min, C 0 = 20 mg L −1 , applied voltage of −1.2 V vs. saturated calomel electrode (SCE)). Furthermore, the dechlorination efficiencies of Co P/O for CAP and TAP reached to 98.7 and 74.2%, respectively. The electron spin resonance and in situ Raman characterizations confirmed that atomic H* was produced via the Co P and the formation of Co Cl bonds occurred on the Co O in Co P/O. The Co Cl bond formation could trap HA molecules onto Co P/O and weaken the C Cl bond strength. The synergistic effect of H* attack and Co Cl bond was responsible for the high dechlorination efficiency. This study offers new insights into the interface mechanism of electroreductive dehalogenation process, and shows a great potential for the remediation of halogenated antibiotics contaminated wastewater.
研究领域:
环境科学
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电化学
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催化科学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Xiao-Cheng Liu,Chuan-Shu He,Zi-Yang Shen,Wen-Qiang Li,Ning Chen,Jun-Sheng Song,Xiao-Guo Zhou,Yang Mu
Fe(III) chelate reduction is of great importance in the homogeneous neutral electro-Fenton (EF) process, but its reduction mechanisms with different reductive species remain unclear. In this study, the reduction mechanisms of several typical Fe(III) chelates through electron and atomic H* were investigated using experiments and density functional theory calculations. The results indicated that the electron reduction efficiencies for [Fe(III)-EDTA] − and [Fe(III)-EDDS] − chelates were 16.23 and 8.31 times higher compared to [Fe(H 2 O) 6 ] 3+ , which was featured by low E LUMO - HOMO and concentrated LUMO distribution around Fe atom. In contrast, the atomic H* reduction efficiency for [Fe(III)-HA] 3+ chelate was 10 times higher than that of electron, attributed to high chelation ability of HA and negative energy barrier of [Fe(III)-HA] 3+ reduction in the atomic H*-dominated system. Additionally, phthalocyanine (Pc) had insignificant effect on pollutant degradation efficiency in the neutral EF systems due to the lower chelate ability of Pc with Fe(III) compared to H 2 O.
研究领域:
环境科学
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化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
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2024
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IF 7.7
Lan-Ying Liu,Min-Hua Cui,John Justo Ambuchi,Shi-Ming Niu,Xin-Hui Li,Wo-Long Wang,He Liu,Guo-Shuai Liu,Ai-Jie Wang
Electrocatalytic hydrodechlorination (EHDC) is a promising approach to safely remove halogenated emerging contaminants (HECs) pollutants. However, sluggish production dynamics of adsorbed atomic H (H* ads ) limit the applicability of this green process. In this study, bimetallic Pd–Cu@MXene catalysts were synthesized to achieve highly efficient removal of HECs. The alloy electrode (Pd–Cu@MX/CC) exhibited better EHDC performance in comparison to Pd@MX/CC electrode, resulting in diclofenac degradation efficiency of 93.3 ± 0.1%. The characterization analysis revealed that the Pd 0 /Pd II ratio decreased by forming bimetallic Pd–Cu alloy. Density functional theory calculations further demonstrated the electronic configuration modulation of the Pd–Cu@MXene catalysts, optimizing binging energies for H* and thereby facilitating H* ads production and tuning the reduction capability of H* ads . Noteably, the amounts and reduction potential of H* ads for Pd–Cu@MXene catalysts were 1.5 times higher and 0.37 eV lower than those observed for the mono Pd electrode. Hence, the introduction of Cu into the Pd catalyst optimized the dynamics of H* ads production, thereby conferring significant advantages to EHDC reactions. This augmentation was underscored by the successful application of the alloy catalysts supported by MXene in EHDC experiments involving other HECs, which represented a new paradigm for EHDC for efficient recalcitrant pollutant removal by H* ads .
研究领域:
环境科学
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材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2019
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IF 7.149
Xiao-Cheng Liu,Wen-Qiang Li,Yi-Ran Wang,Guan-Nan Zhou,Yi-Xuan Wang,Chuan-Shu He,Gong-Ming Wang,Yang Mu
Promotion of iron solubility using ligands is the preliminary step in the homogeneous electro-Fenton (EF) process at a mild pH, but the chelate efficiencies of most organic ligands are unsatisfactory, resulting in insufficient Fe(II) availability. In this study, atomic H* was, for the first time, introduced to the EF process to accelerate the regeneration of the Fe(II)-complex at a mild pH using a Ni-deposited carbon felt (Ni-CF) cathode. The introduction of atomic H* significantly elevated total organic carbon (TOC) abatement of ciprofloxacin (CIP) from 42% (CF) to 81% (Ni-CF) at a natural pH. In the presence of humic acids (HAs), atomic H* introduced via Ni-CF enhanced the CIP degradation rate to 10 times that of the CF at a mild pH. The electron spin resonance (ESR), density functional theory (DFT) calculations, electrochemical characterization, and in situ electrochemical Raman study clearly demonstrated that the atomic H* generated from the Ni-CF cathode was highly efficient at reducing Fe(III)-complexes at a natural pH. Additionally, the Ni-CF could generate atomic H* without significant nickel leaching. Thus, the atomic H* could continuously facilitate iron cycling and, consequently, enhance pollutant mineralization via the homogeneous EF process at a mild pH in an environmentally friendly manner.
研究领域:
环境科学
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化学工程
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水处理
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电化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yun-fei Zhang,Chun-hui Zhang,Yu-feng Liu,Dan Li,Jian-hui Xu,Lei Li,Qi Wu,Jin-hong Fan,Lu-ming Ma
Herein, the SiC-Fe 0 powders were mechanically synthesized and employed for activation of peroxymonosulfate (PMS) to remove florfenicol (FLO). Compared to Fe 0 /PMS system, up to a 3.97-fold increase in degradation rates of 20 mg/L FLO was observed by 25% ( w / w ) SiC-Fe 0 /PMS system in 5 mins, which could be attributed to the increased specific surface area and electron transfer rate of SiC-Fe 0 . Both the radical and non-radical processes were involved in the SiC-Fe 0 /PMS system, in which 1 O 2 and • O 2 − played the dominant role in the FLO degradation and SO 4 •− as well as • OH also participated in the system. ROSs investigation suggested that 1 O 2 , • O 2 − , SO 4 •− were mainly generated from the decomposition of PMS and • OH was mainly derived from the ZVI (or Fe 2+ )-catalyzed activation of O 2 . Meanwhile, H* has a nonnegligible role in PMS activation or the transformation of iron species. Five intermediates of FLO in SiC-Fe 0 /PMS system were identified and a significant removal of the overall toxicity was observed. The degradation pathways of FLO were proposed to be hydrolysis, hydroxylation and dechlorination. Besides, this SiC-Fe 0 /PMS system shows effective removal rate for 2-chlorophenol, acetaminophen, tetrabromobisphenol A and carbamazepine, and the FLO-polluted surface water and artificial wastewater. Overall, this study demonstrated that SiC-Fe 0 was promising in practical application and provided new insights into the generation mechanisms of ROSs in the ZVI/PMS system.
研究领域:
环境科学
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化学工程
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水处理
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高级氧化工艺
✓ 已验证
产品关联
DOI
高影响因子
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