Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 45
·24065-24074
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IF 11.301
Weisheng Yang,Xiu Wang,Liang Jiao,Huiyang Bian,Yongzheng Qiao,Hongqi Dai
Lignin, a renewable and low-cost biopolymer, has been widely reported as an energy-storage material. The energy-storage capability of lignin primarily originates from the redox of its internal quinone group. Hence, effective optimization of the lignin structure is of great significance for increasing the quinone group content, which is vital for improving the energy-storage performance of lignin-based electrode materials. Herein, synthetic polymers (SPs) with an extremely high quinone group content were prepared using lignin-derived aromatic monomers (LDAMs) as precursors. The chemical structure of the SP samples was analyzed using 13C and 31P NMR, and the results showed that their quinone content was as high as 5.49–6.75 mmol g−1, which is 6–7 times higher than that of commercial kraft lignin (KL). The RGO/SP composite was prepared using ultrasound-assisted self-assembly, and as expected, the SP coupled with reduced graphene oxide acquired a high specific capacitance of 352–465 F g−1, which is 1.4–1.9 times higher than that of RGO/KL. In addition, the RGO/SP electrodes showed an excellent rate performance of 265–365 F g−1 at 10 A g−1. Overall, our strategy provides a possibility for the preparation of high-performance lignin-based energy-storage materials.
研究领域:
材料科学
·
能源化学
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DOI
高影响因子
Environmental Science-Processes & Impacts
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2020
·Vol. 22
·期 9
·1898-1907
·
IF 3.238
Shujun Yin,Chenhui Wei,Dongqiang Zhu
Understanding the mechanisms controlling the redox transformation of organic contaminants mediated by biochar is of great significance for application of biochar in remediation of contaminated soils and sediments. Here we investigated the mediation effect of a pine wood-derived biochar (P-char) in comparison with multiwalled carbon nanotubes (MCNTs) and graphite on the reductive dechlorination of hexachloroethane by sulfide. Upon normalization of the mediator's surface area, the reduction rate of hexachloroethane follows an order of P-char < MCNTs < graphite. Aqueous polysulfides and polysulfide free radicals were readily produced by reacting sulfide only with P-char, and the supernatant separated from the reaction system could account for 83.4% of the pseudo-kinetic rate constant of hexachloroethane mediated by P-char. In contrast, MCNTs and graphite had weak abilities to produce reactive sulfur species, and the supernatant exhibited very low reduction capability (<20.7%) of hexachloroethane. Electron paramagnetic resonance (EPR) analysis demonstrated that the surface quinone moieties on P-char induced the formation of polysulfides and polysulfide free radicals from sulfide by serving as one-electron acceptors. Consistently, polysulfides prepared by reacting elemental sulfur with sulfide showed much stronger reducing capability compared to sulfide. Thus, the mediation effect of P-char was dominantly attributed to the surface quinone-induced formation of reactive reducing sulfur species, whereas the mediation effect of MCNTs and graphite mainly stemmed from the enhanced electron transfer by the graphitized carbon. These results showed for the first time that surface quinone-induced formation of aqueous reactive sulfur species could control biochar-mediated reductive dechlorination of chloroorganic contaminants by sulfides.
研究领域:
环境科学
·
污染修复
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiangcheng Zhang,Jingzhen Zhang,Jie Miao,Xue Wen,Chao Chen,Baoxue Zhou,Mingce Long
Photocatalytic H 2 O 2 production is a promising strategy for decentralized applications, but to realize efficient H 2 O 2 production in the ambient conditions and absence of organic sacrifice remains challengeable. Herein, anthraquinone functionalized covalent organic frameworks (TpAQ-COFs) were fabricated by β-ketoenamines links of 2,6-diaminoanthraquinone (AQ) and 2, 4, 6-triformylphloroglucinol (Tp), and the structures and compositions were tuned by controlling the condensation time. The increase of time favors the assembly of TpAQ-COFs into more ordered lamellar stacking structure, and induces the increase of enol-imine form. The critical role of anthraquinone moieties as the active sites for oxygen reduction was proved, that is, facilitating charge separation and enhancing the activity and selectivity of H 2 O 2 production. Upon visible light irradiation, the TpAQ-COF synthesized after 12 h reaction has the highest content of anthraquinone moieties and the best performance for H 2 O 2 production (420 μmol h −1 g −1 ) in the absence of organic sacrificial agents. These findings bring insights to incorporate anthraquinone chemistry into photocatalysts at molecular levels for efficient H 2 O 2 production.
研究领域:
材料科学
·
环境科学
·
化学
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产品关联
DOI
高影响因子
SOLAR ENERGY MATERIALS AND SOLAR CELLS
·
2021
·
IF 7.267
Shanxin Xiong,Yukun Zhang,Jiaojiao Zhang,Xiaoqin Wang,Jia Chu,Runlan Zhang,Ming Gong,Bohua Wu,Guoquan Liu,Wen Luo,Jianwei Xu
Two-dimension covalent organic frameworks (2D COFs) are porous materials with the interlayer π-π interaction and excellent optoelectronic properties. Their adjustable porous structure and designable molecular structure endow them unlimited possibilities in the field of optoelectronic materials and other functional materials . In this paper, 2D COF electrochromic films were prepared by solvothermal synthesis method with different amounts of functionalized carbon nanotubes (FCNT) loading to improve their conductivity. The morphology characterization of COF DAAQ-TFP reveals its intertwined nanofiber structure. The electrochromic performance of COF DAAQ-TFP film shows that the color of COF DAAQ-TFP and FCNT-COF DAAQ-TFP have a reversible transformation from orange to dark brown during the redox process . When the loading amount of FCNT is 1%, FCNT-COF DAAQ-TFP exhibits best electrochromic properties, which has a contrast of 0.358 and coloring time of 5.7 s. Relative to COFs, FCNT-COF has enhanced contrast and stability, which is a potential electrochromic material in many fields such as smart window and smartphone back case.
研究领域:
材料科学
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电化学
·
纳米技术
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2021
·
IF 5.645
Weisheng Yang,Yifei Qu,Bingjie Zhou,Chang Li,Liang Jiao,Hongqi Dai
Lignin-derived aromatic oligomers (LDAOs) are the primary components of lignin depolymerization products. They are typically utilized as renewable crosslinking agents or resin materials with a considerably lower application value than aromatic monomers. Notably, LDAOs are rich in quinone groups, which enable storage and release of charges. In this work, the feasibility of LDAOs as renewable charge storage materials was investigated. LDAOs were first reacted with formaldehyde to generate a synthetic polymer (SP-AOF) via a phenol-formaldehyde condensation reaction. SP-AOF was subsequently incorporated with reduced graphene oxide (rGO), namely rGO/SP-AOF. As expected, the hybrid electrode exhibited high specific capacitance (250 F/g), which was approximately three times higher than that of rGO (87 F/g). This was due to the presence of quinone groups in SP-AOF, which could contribute to the overall capacitance with pseudocapacitance. Moreover, the hybrid electrode was able to deliver a high specific capacitance of 210 F/g even at a high specific current of 10 A/g. 1 H− 13 C heteronuclear single quantum coherence nuclear magnetic resonance (2D HSQC NMR) and phosphorus nuclear magnetic resonance spectroscopy ( 31 P NMR) analyses revealed that SP-AOF displayed higher quinone content (3.76 mmol/g) than commercially available lignin (organosolv and alkali lignin), which resulted in higher energy storage performance. This study provides a promising strategy for the utilization of aromatic oligomers as raw materials to manufacture high-performance lignin-derived energy storage materials.
研究领域:
能源材料科学
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可再生资源利用
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有机化学
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产品关联
DOI
高影响因子
CHEMICAL GEOLOGY
·
2018
·
IF 3.57
Yong Yuan,Xixi Cai,Bin Tan,Shungui Zhou,Baoshan Xing
Solid-phase humic substances (also termed humins, HMs) are the largest fraction of humic substances (HSs) in soils and sediments, which are recently shown to be capable of mediating electron transfer in many key biogeochemical processes. However, the redox properties of HMs remains poorly investigated, likely due to their structural complexity and the lack of efficient methodology. Herein, an electrochemical in situ FITR spectroscopic (EC-FTIRS) technique coupled with two-dimensional correlation spectroscopy (2D-COS) was employed for the first time to study the redox process of complex HMs at a molecular level. In situ FTIR identified that the IR bands of quinone and phenolic moieties in the HMs were potential dependent, suggesting that they were the main redox sites in response to the redox transformation of the HMs. Meanwhile, In situ FTIR characterizations showed that the significant variations in IR bands positioned at ~1500 and ~1470 cm −1 in response to the applied potentials, providing evidence for the presence of quinone radical and dianion intermediates during the redox process. The 2D-COS analysis was used to further explore variations in infrared intensities as a function of the potentials applied to reduce or oxidize the HMs, which indicated the occurrence of the typical redox reactions of quinone in the HMs. These results improve our understanding on the redox mechanism of HMs at the molecular level and have significant implication for in-depth understanding of biogeochemical processes.
研究领域:
环境科学
·
分子生物学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Jiahang Liu,Yingying Chu,Xiaoyang Li,Mengying Qian,Weiming Zhang
The co-catalytic effect of hydroquinone/quinone electron shuttle has received great attention in the area of Fenton-like reaction. However, the crucial roles of phenolic or hydroquinone moieties in the chemical structures of organic pollutants have always been overlooked. In this study, we discovered that the introduction of rifampicin (RIF), a representative of rifamycin antibiotics, could trigger complete degradation of atrazine (ATZ) in the Fe(III)/H 2 O 2 system. By exploring the influences of initial Fe(III), H 2 O 2 , RIF concentrations and pH values on ATZ degradation efficiency, key components affecting metal ion valence transitions in the system were identified. Quenching experiments, probe tests and EPR analysis verified that •OH served as the primary active species, while HO 2 •/O 2 •− was also generated. Through monitoring Fe(II) concentration variations and employing mass spectrometric analyses, the oxidation pathway of RIF was elucidated: When mixed with Fe(III), the naphthohydroquinone moiety of RIF immediately acted as a direct electron donor to reduce Fe(III) to Fe(II), while itself being oxidized to RIF-Q. Upon H 2 O 2 addition, it rapidly triggered the classical Fenton reaction with Fe(II) to generate •OH, enabling ATZ degradation. Simultaneously, RIF-Q underwent further oxidative breakdown, with some degradation products retaining the capacity to continuously donate electrons to Fe(III), thereby promoting its reduction. This study provides new insights for the co-catalytic effect of pollutant-derived electron shuttles on the transition of metal ion valences.
研究领域:
环境化学
·
污染物降解
·
高级氧化过程
·
金属离子价态转化
·
有机污染物转化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Biomaterials Science & Engineering
·
2022
·
IF 5.395
Hanyin Zhu,Yongyi Qu,Shuai Wang,Jixi Huang,Jing Zhu,Lu Wang,Kaiyong Cai,Jixi Zhang
The elevation of antioxidant defense systems by adaptation response to localized reactive oxygen species (ROS) accumulation may confer resistance to excessive oxidative stress and cause therapeutic lethality. Herein, a highly effective tumor therapy is developed through perturbation in cellular redox homeostasis. Specifically, metal-ion-assisted oxidation polymerization of the melanin precursor (l-DOPA) whose carboxyl groups exert a charge-shielding effect leads to the formation of catechol-rich but quinone-deficient nanoparticles (NPs). These NPs possess appreciable ROS-scavenging ability, and particularly the raised quinone group levels in oxidized products can then trigger subsequent depletion of antioxidative species (GSH) and, in turn, the redox-cycle consumption of catechol/quinone groups. After incubating with cells, varying degrees of redox-state and energy metabolism fluctuations with time (∼6 h) are observed, where ROS/GSH levels rebound to a maximum peak (up to ∼280%) higher than the normal redox state after hitting the bottom within a short time (1 h). Notably, systematically triggered redox stress response can sensitize cells to an extremely endangered metastable state. The synergy of temporally photoactivated thermal stress can produce overwhelming oxidative stress, thus leading to significant inhibition of cancer cells. This work established a new paradigm of redox perturbator-based programed and combined cancer therapy.
研究领域:
癌症治疗
·
纳米技术
·
氧化还原生物学
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光热治疗
·
肿瘤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）