Science Advances
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2024
·Vol. 10
·期 24
·
IF 11.7
Xinliang Li,Yanlei Wang,Junfeng Lu,Pei Li,Zhaodong Huang,Guojin Liang,Hongyan He,Chunyi Zhi
Despite their potential as conversion-type energy storage technologies, the performance of static lithium-bromide (SLB) batteries has remained stagnant for decades. Progress has been hindered by the intrinsic liquid-liquid redox mode and single-electron transfer of these batteries. Here, we developed a high-performance SLB battery based on the active bromine salt cathode and the two-electron transfer chemistry with a Br−/Br+ redox couple by electrolyte tailoring. The introduction of NO3− improved the reversible single-electron transition of Br−, and more impressively, the coordinated Cl− anions activated the Br+ conversion to provide an additional electron transfer. A voltage plateau was observed at 3.8 V, and the discharge capacity and energy density were increased by 142 and 159% compared to the one-electron reaction benchmark. This two-step conversion mechanism exhibited excellent stability, with the battery functioning for 1000 cycles. These performances already approach the state of the art of currently established Li-halogen batteries. We consider the established two-electron redox mechanism highly exemplary for diversified halogen batteries.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
OPTICAL MATERIALS
·
2021
·
IF 3.08
Rui Qu,Mingyang Gao,Haonan Li,Xiaofei Qi,Cheng Liu,Wu Zhao,Junfeng Yan,Zhiyong Zhang
Formamidinium lead bromide perovskite (FAPbBr 3 ) nanostructures have aroused increasing attention considering their excellent optoelectronic performance and higher stability than their MA- and Cs-based counterparts. Herein, we synthesized size-tunable FAPbBr 3 quantum dots (QDs) at room temperature. The size of the perovskite QDs could be ajusted from 5.4 to 2.3 nm by just varying the amount of Hydrobromic Acid (HBr) added into the precursor. As a result, the photoluminescence (PL) emissions exhibited large blueshift from 531 to 446 nm due to quantum confinement effect. Quantum mechanical calculations of the optical gap fitted well with the experimental results. We found that the addition of HBr not only increased the concentration of the Br − but also protonated the oleylamine ligands. The two events synergically governed the size-decreasing effect of the QDs with increasing amount of HBr. The size-tunable FAPbBr 3 QDs showed great application prospect in the field of photoelectric devices.
研究领域:
材料科学
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光学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Liang Zhang,Zhen Ma,Haidong Sun,Rongzi Zhang,Zilong Zhao,Jie Wang,Zhonglin Zhang,Zhong Liu,Jun Li,Xiao Du,Xiaogang Hao
Based on the superior selectivity of bismuth oxybromide (BiOBr) for Br - , the excellent electrical conductivity of carbon nanotubes (CNTs), and the ion exchange capacity of quaternized chitosan (QCS), a three-dimensional network composite membrane electrode CNTs/QCS/BiOBr was constructed, in which BiOBr served as the storage space for Br - , CNTs provided the electron transfer pathway, and QCS cross-linked by glutaraldehyde (GA) was used for ion transfer. The CNTs/QCS/BiOBr composite membrane exhibits superior conductivity after the introduction of the polymer electrolyte, which is seven orders of magnitude higher than that of conventional ion-exchange membranes. Furthermore, the addition of the electroactive material BiOBr improved the adsorption capacity for Br - by a factor of 2.7 in electrochemically switched ion exchange (ESIX) system. Meanwhile, the CNTs/QCS/BiOBr composite membrane displays excellent Br - selectivity in mixed solutions of Br - , Cl - , SO 4 2- and NO 3 – . Therein, the covalent bond cross-linking within the CNTs/QCS/BiOBr composite membrane endows it great electrochemical stability. The synergistic adsorption mechanism of the CNTs/QCS/BiOBr composite membrane provides a new direction for achieving more efficient ion separation.
研究领域:
材料科学
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环境工程
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Mingge Wu,Qianqian Li,Cheng Chen,Guijin Su,Maoyong Song,Bohua Sun,Jing Meng,Bin Shi
The high-efficiency photocatalytic debromination of hexabromocyclododecane (HBCD) as new POPs and discovery of involved mechanisms remain a challenge. Herein, challenging Pd-anchored hollow-rod-like-g-C 3 N 4 (Pd/HR-g-C 3 N 4 ) was constructed as visible-light-driven photocatalyst. Complete destruction of (±)-α, (±)-β and (±)-γ-HBCD with 92.6 % bromine-removal was achieved at 60 min in optimal system of anaerobic methanol-water (70:30) mixture with 0.5 % Pd/HR-g-C 3 N 4 , being superior to most studied HBCD catalytic systems. The higher photocatalytic reduction performance is contributed to enhanced photoexcited-carriers separation and more negative conduction band arising from distinctive 1D-cavity of HR-g-C 3 N 4 , and surface-atomically dispersed Pd. A never-reported degradation pathway in which hydrodebromination and addition ring-opening synergistically occur is proposed according to identified products of ten saturated chain alkanes, C 12 H 19 Br 5 and C 12 H 19 Br 7 . Ulteriorly, hydride-transfer resulted in rapid hydrodebromination of HBCD over Pd/HR-g-C 3 N 4 , where H chiefly derives from methanol instead of water although they synergistically promoted e − utilization. This provided a valuable sight into the cost-effective pollution-removal of HBCD.
研究领域:
环境科学
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化学工程
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材料科学
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催化
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DOI
高影响因子
CHEMOSPHERE
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2019
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IF 5.108
Yuting Jiang,Shiying Yang,Junqin Liu,Tengfei Ren,Yixuan Zhang,Xinrong Sun
Hexabromocyclododecane (HBCD) has been listed in Annex A of the Stockholm Convention on Persistent Organic Pollutants (POPs) in 2013, but till now there is a lack of efficient methods for its degradation. In this study, nanoscale zero-valent aluminum (nZVAl), an excellent reductant with a very low redox potential of E 0 (Al 3+ /Al 0 ) = −1.662 V and strong electron transfer ability, was used to reductively degrade HBCD. Nearly 100% HBCD was degraded within 8 h reaction at 25 °C in ethanol/water (v/v, 50/50) solution without pH adjustment. And about 67% cyclododecatriene (CDT) was obtained, which is the complete debromination product. What’s more, the yield of Br − could achieve nearly 100% after optimizing conditions. The reaction was strongly promoted by increasing the dosages of nZVAl or decreasing the initial concentration of HBCD. The temperature had the most significant influence and the degradation was completed in 40 min with elevating the reaction temperature to 45 °C. The reaction mechanism was further revealed through the characterization of nZVAl particles before and after the reaction by SEM-EDS, TEM , HRTEM , XRD, and XPS. It was found that, after corrosion of the oxide film on the surface of nZVAl, metallic aluminum inside was exposed. The reactive sites were provided and electrons released were transferred from nZVAl to HBCD, causing HBCD degraded to dibromocyclododecadiene (DBCD) and then CDT by reductive debromination. These findings imply that nZVAl can degrade HBCD efficiently with no extra energy input and this offers a new idea for better treatment of HBCD.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
DESALINATION
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2024
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IF 8.3
Xu Yin,Renping Li,Wei Li,Zhifeng Gao,Kajia Wei,Hongwei Zhu,Liankai Gu,Yun Jiang,Weiqing Han
Br − -containing wastewater has the risk of increasing Br − levels in receiving bodies if released into aquatic environments. Electrochemical oxidation is regarded as an ideal method for Br − removal and Br 2 extraction because of its simple procedure and high efficiency. In this work, a novel oxygen vacancy enriched Ti/O v -Co 3 O 4 -NRs electrode was fabricated and used for Br − removal and Br 2 extraction in Br − -containing wastewater. Characterization and experimental results showed that the Ti/O v -Co 3 O 4 -NRs electrode has more prominent bromine evolution reaction (BER) performance than several commercial electrodes (graphite, Ti/RuO 2 -Ir, Ti/PbO 2, etc.). Notably, the construction of oxygen vacancies obviously accelerated the removal of Br − (53 % improvement) by facilitating Br − adsorption and electron transfer. In addition, the influence factors such as initial pH, initial Br − concentration, current density, coexisting ions and temperature on Br − removal were optimized. The Ti/O v -Co 3 O 4 -NRs electrode also exhibited highly stable catalytic activity and conductivity. After 10 cycles, the removal rate of Br − decreased by 2.20 %, and the yield of Br 2 decreased by 3.6 %. In actual applications, the unit energy consumption reached 1.59–1.76 kJ·g −1 Br, and the current efficiency remained above 70 % throughout the whole treatment process. In addition, >80 % of the TOC could be removed during Br 2 extraction, which was more acceptable than the current reported experimental value of electrochemical Br 2 extraction and exhibited great application prospects.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2024
·Vol. 46
·期 2
·1-13
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IF 3.2
Wang Tao,Deng Lin,Dai Wenjuan,Tan Chaoqun,Hu Jun,Singh Rajendra Prasad
Brominated halonitromethanes (Br-HNMs) are generated in water disinfection processes and present high toxicity to human health. This work used aspartic acid (ASP) as the precursor to reveal that bromide (Br − ) induced the production of Br-HNMs in the UV/chlorine disinfection process. Consequently, six Br-HNMs were identified, and their yields presented an increasing and then declining evolution over the reaction time from 0 to 15 min. Also, the total Br-HNMs yield reached the maximum of 251.1 μg L −1 at 5 min and then declined to 107.1 μg L −1 . The total Br-HNMs yield increased from 2.40 to 251.14 μg L −1 with the increase of Cl 2 :Br − ratios from 0.25 to 3.0 by increasing free chlorine dosage with a fixed Br − concentration, and it increased from 207.59 to 251.14 μg L −1 and then decreased to 93.44 μg L −1 with the increase of Cl 2 :Br − ratio from 1.0 to 3.6 by increasing Br − concentration with a fixed free chlorine dosage. Besides, the total Br-HNMs yield reached the highest value (251.14 μg L −1 ) at pH 7.0 and the lowest value (74.20 μg L −1 ) at pH 8.0. Subsequently, the possible reaction mechanism of Br-HNMs generated from ASP was deduced, and the changes in toxicity of Br-HNMs also followed an increasing and then declining trend, closely relating to Br-HNMs yields and Br − utilization. This work explored and illustrated the yields, influence factors, reaction mechanisms, and toxicity of Br-HNMs formed from Br − containing ASP water during UV/chlorine disinfection, which might help to control Br-HNMs formation.
研究领域:
环境科学
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水处理工程
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毒理学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
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IF 10.8
Yaohua Wu,Huazhe Wang,Juanshan Du,Yi Hu,Qinglian Wu,Wanqian Guo,Wonyong Choi
This study demonstrates that the oxidation of bromide by birnessite (δ-MnO2) results in the concurrent production of soluble manganese (Mn(II)) and reactive bromine (RBr) species in frozen solutions, a process not observed in aqueous solutions. This enhanced oxidation in ice is attributed to the concentration of protons, birnessite, or bromide in the ice grain boundary region. Furthermore, different types of commercial manganese oxides can also oxidize bromide to RBr and release Mn(II) in ice. The presence of fulvic acid (FA) further increases the simultaneous production of RBr and Mn(II) in ice, accompanying the formation of organobromine compounds (OBCs). In frozen δ-MnO2/Br–/FA system, a significant increase in OBCs, mainly highly unsaturated and phenolic compounds, was detected using Fourier transform ion cyclotron resonance mass spectrometry. A marked contrast was observed in the number of OBCs formed in frozen solutions (853 and 415 OBCs at initial pH 3.0 and 5.8, respectively) compared to their aqueous counterparts (11 and 23 OBCs). These findings introduce a new pathway for the formation of RBr, Mn(II), and OBCs in ice, highlighting the need for further research on the environmental fate of bromide and manganese.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
·
IF 5.589
Rui Wang,Ting Tang,Guining Lu,Zhiqiang Zheng,Kaibo Huang,Huafeng Li,Xueqin Tao,Hua Yin,Zhenqing Shi,Zhang Lin,Fengchang Wu,Zhi Dang
This study investigated the relative significance of electron transfer (e-transfer) and H-atom transfer (H-transfer) in a nanoscale zerovalent iron (n-ZVI) system and six n-ZVI-based bimetallic systems (Fe/Cu, Fe/Ni, Fe/Pd, Fe/Ag, Fe/Pt, and Fe/Au) through a case study of the debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47). The results revealed that the reactivities of these bimetallic particles to BDE-47 decreased in the following order: Fe/Pd > Fe/Ag > Fe/Cu > Fe/Ni > Fe/Au > Fe/Pt ≈ n-ZVI. Debromination of BDE-47 in metal-H 2 systems suggested that Ni, Pd, Pt, Cu and Au can utilize H 2 to debrominate BDE-47. In the H-transfer process, BDE-47 preferentially debrominated the para‑ bromine substituent to generate BDE-17, whereas in the e-transfer process, BDE-47 preferentially debrominate ortho‑ bromine substituent to generate BDE-28. The debromination pathways of BDE-47 in bimetallic and NaBH 4 -metal systems suggested that Fe/Ni, Fe/Pd and Fe/Pt debrominate polybrominated diphenyl ethers (PBDEs) through a H-transfer dominant mechanism, while Fe/Ag debrominate PBDEs through an e-transfer dominant mechanism. In the cases of Fe/Cu and Fe/Au, the e-transfer and H-transfer may be equally involved in the debromination of PBDEs. These results greatly improve our understanding of the relative significance of e-transfer and H-transfer in the dehalogenation of halogenated aromatic compounds (HACs) in various n-ZVI-based bimetallic systems.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
·
IF 10.753
Xin-Yang Zhang,Ye Du,Yao Lu,Wen-Long Wang,Qian-Yuan Wu
Ozonation plays an important role in wastewater treatment for reuse. However, the toxicity of wastewater treated with ozone considerably increases with bromide (Br − ) concentration >100 μg/L. Nine newly identified brominated disinfection byproducts (Br-DBPs) that are highly toxic in ozonated Br − -containing wastewater were found in our recent work, including 2-bromostyrene, 1-bromo-1-phenylethylene, 2-bromobenzaldehyde, 3-bromobenzaldehyde, 4-bromobenzaldehyde, 2-bromophenylacetonitrile, 3-bromophenylacetonitrile, 4-bromophenylacetonitrile, and 2,4,6-tribromophenol. In the present study, the formation and calculated toxicity index of the nine newly identified Br-DBPs were evaluated. The correlations between the water quality index and the formation of nine Br-DBPs were also analyzed. With the increase of ozone dosage, the concentrations of bromostyrenes, 3-bromobenzaldehyde, 4-bromobenzaldehyde, 2-bromophenylacetonitrile, and 2,4,6-tribromophenyl in the ozonated samples gradually increased. With the increase of Br − concentration, the concentrations of bromostyrene, 2-bromobenzaldehyde, and 2,4,6-tribromophenol gradually increased. With the increase of NH 4 + concentration, the concentrations of bromophenylacetonitriles gradually increased. Among the nine Br-DBPs, the bromophenylacetonitriles and 2,4,6-tribromophenol contributed the most to the cytotoxicity index, 2,4,6-tribromophenol and bromostyrenes contributed the most to the genotoxicity index, and bromophenylacetonitriles and bromostyrenes contributed the most to the oxidative damage index. The dissolved organic carbon levels strongly correlated with the formation of 3-bromophenylacetonitrile and 4-bromophenylacetonitrile, and the fluorescence I–V region intensity integral was correlated with the formation of 4-bromobenzaldehyde and 2,4,6-tribromophenol. The results of the present study clarified the formation potential of the nine widely existing newly identified Br-DBPs, confirmed the high calculated toxicity indices, and are of great value for future research on Br-DBPs.
研究领域:
环境科学
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毒理学
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产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Xiao-Qiu Lin,Jia-Mei You,Ling-Yu Meng,Naoko Yoshida,Jing-Long Han,Cong-Ju Li,Ai-Jie Wang,Zhi-Ling Li
Tetrabromobisphenol A (TBBPA), a hazardous and persistent flame retardant , has been widely detected in the natural aquatic system. The acceleration of reductive debromination (rate-limiting process) is vital during the decomposition and detoxification of TBBPA. This study achieved superior TBBPA electrochemical reductive debromination performance by nano Pd doped Ni foam electrode (4.8 times higher than Ni foam electrode). The optimal TBBPA reductive debromination performance was obtained under −1.2 V of cathode potential, 1.2 wt% of Pd loading, 10 mg L −1 of TBBPA and 100 mM of Na 2 SO 4 as the electrolyte solution. UPLC-QTOF-MS verified that Br atoms in TBBPA were removed sequentially to form bisphenol A as the major product. Most TBBPA was reductively debrominated by atomic H* through indirect hydrodebromination, evidenced by the atomic H* quenching test. The higher solution conductivity and appropriate TBBPA concentration would contribute to the debromination efficiency. Excessive H 2 generation whether by over negative potential or H atom richness electrolyte largely disturbed the reaction process and restricted the debromination. The improved generation of reductant (H*) ads Pd was the most significant, while excessive Pd loading would make aggregation and limit the debromination efficiency. The study confirmed the optimization strategies of conditions for Pd/Ni foam electrode and revealed the related function mechanism for stimulating TBBPA electrochemical reduction, giving suggestions for the efficient removal of TBBPA in the aquatic environment.
研究领域:
环境科学
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电化学
·
污染控制
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DOI
PubMed
高影响因子
CHINESE CHEMICAL LETTERS
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2022
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IF 8.455
Jingxin Yang,Hongrui Ma,Chuan Wang,Hong Liu
Bromate formation has been found in the SO 4 •− -based oxidation processes, but previous studies primarily focused on the bromate formation in the homogeneous SO 4 •− -based oxidation processes. The kinetics and mechanisms of bromate formation are poorly understood in the heterogeneous SO 4 •− -based oxidation processes, although which have been widely studied in the eliminations of micropollutants. In this work, we found that the presence of CuO, a common heterogeneous catalyst of peroxymonosulfate (PMS), appreciably enhanced the bromate formation from the oxidation of bromide by PMS. The conversion ratio of bromide to bromate achieved over 85% within 10 min in this process. CuO was demonstrated to play a multiple role in the bromate formation: (1) catalyzed PMS to generate SO 4 •− , which then oxidizes bromide to bromate; (2) catalyzed the formed free bromine to disproportionate to bromate; (3) catalyzed the formed free bromine to decomposed back into bromide. In the CuO-PMS-Br system, bromate formation increases with increasing CuO dosages, initial CuO and bromide concentrations, but decreases with increasing bicarbonate concentrations. The presence of NOM (natural organic matter) resulted in a lower formed bromate accompanied with organic bromine formation. Notably, CuO catalyzes PMS to transform more than 70% of initial bromide to bromate even after recycled used for six times. The formation of bromate in the PMS catalysis by CuO system was also confirmed in real water.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）