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Energy Storage Materials · 2021 · IF 17.789

Boosting the cyclability of tetracyanoquinodimethane (TCNQ) as cathode material in aqueous battery with high valent cation

Yun Zhong,Yankai Li,Jintao Meng,Xing Lin,Zhimei Huang,Yue Shen,Yunhui Huang

7,7,8,8-tetracyanoquinodimethane (TCNQ) is a low-cost redox active organic compound which has high theoretic specific capacity. But when it is used as cathode material in batteries , it always suffers from fast performance decaying because of material dissolution. In this work, Al 3+ salt is added in a Na 2 SO 4 /ZnSO 4 aqueous electrolyte to stabilize the crystalline structure of TCNQ and depress its solubility. Surprisingly, we found the insertion/extraction of high valent cations (Al 3+ and Zn 2+ ) in TCNQ is highly reversible, which leads to synergistic improvement of both specific capacity and cycle life. The obtained cathode exhibits a reversible capacity of 245.8 mAh g -1 at 0.5 A g -1 and a cycle-life of 1000 rounds at 3 A g -1 . Our work demonstrates that molecular organic electrode materials are very different from conventional inorganic cathode materials in terms of high valent cation intercalation reversibility. Adding high valent cation salts is a simple and effective way to enhance the electrochemical performance of molecular organic electrode materials, and consequently build low cost, high performance aqueous rechargeable batteries.

研究领域: 储能 · 电化学 · 材料科学 · 水系电池 · 有机电极材料
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JOURNAL OF ELECTRONIC MATERIALS · 2024 ·Vol. 53 ·期 5 ·2656-2665 · IF 2.2

Solvothermal Synthesis and Growth of Covalent Organic Framework Electrochromic Film with Triphenylamine Active Unit

Xiong Shanxin,Zhang Yukun,Zhang Wei,Yang Nana,Lv Fengyan,Guo Jingru,Cui Xin,Fang Ke,Chen Min,Wang Chenxu,Hua Chunxia,Zhang Runlan,Chu Jia,Xu Jianwei

Covalent organic frameworks (COFs) with reversible redox units and a conjugated molecular skeleton possess novel photoelectrochemical properties. In this work, tris(4-aminophenyl)amine and 4,4-biphenyldiformaldehyde were chosen to synthesize TABP-COF electrochromic film with triphenylamine (TPA) active unit by a solvothermal method in a Teflon-lined reactor. The growth process and reaction time optimization of the TABP-COF were studied. TABP-COF shows a self-assembly growth process from an array of nanosheets to nanospheres. Owing to the redox characteristics of TPA, the TABP-COF film exhibits reversible electrochromic behavior. With a solvothermal reaction time of 72 h, the TABP-COF-3 film exhibits the best electrochromic properties, including contrast of 0.483 and response time of 7.3 s/13.6 s. Considering the abundance of redox-active units that can be chosen, COF materials with different redox units and color changes can be designed for a variety of applications in the field of electrochromic materials.

研究领域: 材料科学 · 电化学 · 纳米技术 · 有机化学
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CHEMICAL GEOLOGY · 2021 · IF 4.015

Effects of low-molecular-weight organic acids/thiols on hydroxyl radical production from natural siderite oxidation

Hao Yu,Peng Zhang,Jiayu Liu,Yunsong Zheng,Nasiru Abba Mustapha

Oxygenation of siderite produces hydroxyl radicals (•OH) that are capable of transforming the pollutants. Yet, the influence of low-molecular-weight organic acids (LMWOAs)/ thiols (LMWOTs) which are widely occurring in soils and waters on •OH production from the oxygenation process of siderite is poorly understood. Results of this study show that the presence of LMWOAs/LMWOTs significantly facilitated •OH production from siderite oxidation by O 2 at pH 6–8. For instance, at pH 7, the cumulative •OH concentration within 24 h was only 1.3 μM for oxygenation of 1 g/L siderite, while it boosted to 19.7 and 7.2 μM, respectively, with the respective addition of 1 mM ethylenediaminotetraacetate and cysteine. The mechanisms responsible for the enhanced •OH production are associated with the complexation ability and redox activity of LMWOAs/LMWOTs. In the absence of LMWOAs/LMWOTs, •OH is mainly produced from the oxidation of adsorbed Fe(II) by O 2 , followed by the oxidation of structural Fe(II) on siderite surface. In the presence of LMWOAs, LMWOAs react with adsorbed Fe(II) and structural Fe(II) to produce complexed Fe(II). Therefore, the oxidation of LMWOAs complexed Fe(II) by O 2 predominantly contributed to •OH production. Although the complexation ability of LMWOTs is weaker than that of LMOWAs, LMWOTs can reduce O 2 to generate •O 2 − and H 2 O 2 , thus facilitating •OH production. Based on the proposed mechanisms, a kinetic model was developed to quantify the relative contribution of each pathway to •OH production. The addition of 1 mM citrate and cysteine in siderite suspension could increase the removal of trichloroethylene from <5% to 15% and 7%, respectively. Our study reveals the overlooked catalytic effects of LMWOAs/LMWOTs in enhancing •OH production from siderite oxidation by O 2 under redox-dynamic conditions.

CAS / MDL: 5625-37-6
研究领域: 环境科学 · 化学 · 污染控制
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Enhanced selective electrosorption of Pb2+ from complex water on covalent organic framework-reduced graphene oxide nanocomposite

Hao Zhang,Xiaodie Li,Chengming Xiao,Jia Xie,Xin Yan,Chaohai Wang,Yujun Zhou,Junwen Qi,Zhigao Zhu,Xiuyun Sun,Jiansheng Li

Selective capture of the toxic and ubiquitous heavy metal ions is crucially desired yet still significant challenge for water purification. Herein, a covalent organic framework-reduced graphene oxide nanocomposite (TpPa@rGO) was developed and employed as cathode for the first time to selectively remove Pb 2+ from complex water via an electrosorption process. Specifically, the rGO provides the electrical conductivity and induces the electric double layer capacitance to attract cations approaching to the electrode surface, while the TpPa endows abundant highly selective redox-active sites to capture Pb 2+ . Thanks to the ingenious synergy of capacitive rGO and redox-active TpPa, more than 99.6% of Pb 2+ can be effectively removed by the TpPa@rGO electrode in a mixed solution containing Pb(NO 3 ) 2 (50 mg L −1 ) and multicomponent nitrates (100 mg L −1 for each), as well as good cycling stability. Interestingly, the interfering ions can serve as additional electrolytes to accelerate the accumulation of Pb 2+ around the TpPa@rGO electrode instead of competing for active sites, thereby increasing the absolute adsorption capacity of Pb 2+ from 94.6 mg g −1 in single Pb(NO 3 ) 2 solution to 129.8 mg g −1 in the multicomponent solution. The enhanced selective electrosorption mechanism on Pb 2+ removal by TpPa@rGO and their recyclability were also investigated. The capacitive matrix and additional electrolytes accelerate the ion transfer and enhance ion accessibility to the electrode, thereby anchoring the Pb 2+ on the N/O groups of TpPa. This study may put forward a promising method for the selective capture of heavy metal ions in complex water.

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 32 ·期 38 ·2204833 · IF 19.924

Dual Redox Active Sites N-C@Ni2P/NiSe2 Heterostructure Supercapacitor Integrated with Triboelectric Nanogenerator toward Efficient Energy Harvesting and Storage

Xiangyang Gao,Yuanzheng Zhang,Shukun Yin,Yiqian Mao,Jinzheng Gui,Jingxing Li,Yafei Zhao,Chengliang Sun,Shishang Guo

Exploring efficient energy systems with integrated energy harvesting and storage toward sustainable power sources is an extremely promising solution for alleviating the energy crisis but nevertheless remains an arduous challenge. Here, a high-efficient self-charging power system (SCPS) by integrating solid-state asymmetric supercapacitors device (SASD) and rotational triboelectric nanogenerator (RTENG) to achieve efficient energy harvesting and storage is reported. Dual redox active sites Ni 2 P/NiSe 2 heterostructure is homogeneously inlaid on N-C (N-C@Ni 2 P/NiSe 2 ) via an in situ phosphoselenization, which achieves the maximum exposure of active sites and prevents the aggregation of nanoparticles. The ingeniously designed N-C@Ni 2 P/NiSe 2 heterostructure features high activity dual redox sites, well-defined heterointerface, and stable superhighway conductive support, which facilitates high electrochemical reaction efficiency, accelerated reaction kinetics, and enhanced electrochemical stability, thus achieving high capacitance and excellent stability. Meanwhile, the SASD delivers high energy density and long lifespan. Furthermore, the RTENG exhibits high output performance, enabling efficient energy harvesting. The SCPS can reach a voltage of 3.8 V within 40 s, and continuously power electronics. It is believed that the proposed survey based on the design and integration of dual redox active sites heterostructure will offer a new prospect for next-generation sustainable power sources.

研究领域: 材料科学 · 能源存储与转换 · 纳米技术
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JOURNAL OF THE ENERGY INSTITUTE · 2024 · IF 5.6

Composite xNiFe2O4/(1-x)SrFe12O19 oxygen carriers for chemical looping reforming of bioethanol coupled with water splitting to coproduce syngas and hydrogen

Mingxuan Zhong,Chenxuanzi Wang,Jiajun Xu,Yongcheng Cai,Bo Xiao,Tingting Xu,Xun Wang

Sr–Fe oxides are suitable oxygen carriers (OCs) with excellent cyclic stability. However, the moderate redox activity causes a deficiency in H 2 yield in chemical looping reforming coupled with water splitting (CLR-WS) process. Herein, we designed and prepared the composite xNiFe 2 O 4 /(1-x)SrFe 12 O 19 OCs by ball milling method, which exhibited both high redox activity and high cyclic stability during reactions. A series of characterizations showed that the introduction of NiFe 2 O 4 promoted the oxygen vacancy formation and the release of lattice oxygen, facilitating the reforming of bioethanol in fuel reactor (FR). During CLR-WS process, a high carbon conversion of 79.20 % and a H 2 yield of 13.23 mmol/g OC were achieved by 3Ni7Sr OC at 800 °C, outperforming that of the conventional SrFe 12 O 19 OC. Moreover, the severe carbon deposition and sintering issues inherent to NiFe 2 O 4 were avoided due to the presence of Sr. All Sr-containing composite OCs showed H 2 purity exceeding 99.26 % and excellent cycling stability with no apparent activation of oxygen transport capacity over 3000 min redox reactions.

研究领域: 化学工程 · 材料科学 · 能源工程 · 环境工程
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Environmental Technology & Innovation · 2025 · IF 7.1

Micro-electrolytic degradation of rhodamine B by Cu-Fe-Co trimetallic catalysts: Synergistic mechanisms and reaction pathways

Shuzhen Yang,Bingjing Tian,Yanfang Huang,Bingbing Liu,Shengpeng Su,Wenjuan Wang,Guihong Han

The persistent dye rhodamine B (RhB) in textile wastewater poses severe ecological threats, demanding efficient and sustainable treatment technologies. This study synthesized a novel trimetallic Cu-Fe-Co catalyst via a nitrogen-atmosphere co-reduction method. The catalyst’s unique advantage lies in the synergistic effects of Cu, Fe, and Co, which significantly enhance catalytic performance. The redox-active phases of Cu, combined with the Fenton-like reactivity of Fe, are further optimized by Co doping to improve reactive oxygen species (ROS) generation and electron transfer efficiency. Characterization revealed a dendritic structure dominated by Cu, Cu₂O, and FeO phases, with Co-induced lattice expansion (Δ d / d = +0.25 %) enhancing surface reactivity. Under optimized conditions (pH 3, 1.5 g/L catalyst, 20 mg/L RhB), the ternary Cu-Fe-Co catalyst achieved 99.8 % RhB degradation within 40 min, with high mineralization efficiency (46.5 % TOC removal, 82.1 % COD removal). Mechanistic studies demonstrated that Co incorporation promotes the conversion of superoxide radicals (·O₂⁻) into long-lived singlet oxygen (¹O₂), synergistically enhancing oxidative effects from ·OH and ¹O₂, while in situ H₂O₂ generation drives radical chain reactions. Compared to binary catalysts, the ternary system exhibits superior degradation kinetics for RhB and maintains 95.8 % degradation efficiency even after five cycles. This study provides new insights into trimetallic catalyst design, highlighting its practical potential for wastewater treatment.

研究领域: 环境科学 · 催化 · 材料科学 · 化学工程 · 水处理技术
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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

High-Temperature Tolerant Flexible Supercapacitors with Redox-Active Water-in-Salt Hydrogel Electrolytes

Chong Peng,Na Wang,Xinyi Huang,Mingwei Zhao,Siyu Yu

High-temperature-tolerant flexible supercapacitors are essential for powering emerging wearable and portable devices operating under harsh environmental conditions. Conventional hydrogel electrolytes exhibit excellent ionic conductivity, flexibility, and biocompatibility; however, their practical application is hindered by water evaporation at elevated temperatures and a narrow electrochemical window limited by the water decomposition voltage (1.23 V). In this work, we present a novel heat-resistant and redox-active hydrogel electrolyte containing a ZnCl2 water-in-salt solution and a redox-active additive of (NH4)2Fe(SO4)2. The strong coordination between Zn2+ ions and water molecules effectively suppresses water activity, thereby enhancing the thermal stability and expanding the electrochemical window. Furthermore, the incorporation of (NH4)2Fe(SO4)2 contributes to both faradaic charge storage through Fe2+/Fe3+ redox reactions and improved thermal stability via enhanced water coordination. When paired with KOH-activated carbon nanofiber electrodes, a redox electrolyte enhanced flexible supercapacitor has been constructed. The device delivers a wide working voltage of 2.0 V, a high energy density of 23.2 Wh kg–1, and stable operation across a broad temperature range from 0 to 100 °C. This work offers a promising strategy for developing high-performance, thermally stable energy storage devices suitable for next-generation flexible electronics.

CAS / MDL: 9002-89-5
研究领域: 储能 · 材料科学 · 电化学 · 纳米技术 · 柔性电子学
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2025 · IF 7.8

Integrating Experimental Insights with Machine Learning for Inverse Design of Sustainable Lignin-Derived Cr (VI) Adsorbents

Huirong Zhang,Yi Shen,Jinglei Cui,Baofeng Wang,Yanxia Guo,Dongke Zhang,Fangqin Cheng

s Lignin-derived carbonaceous materials have emerged as promising candidates for heavy metal remediation owing to their low cost, tunable surface chemistry, and hierarchical porosity. In this study, a FeCl 3 –urea co-activation strategy was employed to synthesize N-doped hierarchical porous carbons (N-HPCs) from lignin for efficient Cr (VI) removal. The synthesis parameters were systematically optimized using a machine learning (ML) workflow, with experimental data serving as the training set. Gradient boosting regression (GBR) achieved high predictive accuracy (R 2 = 0.86), and SHAP-based feature importance analysis identified pyridinic-N (N-5) content as the dominant factor governing Cr (VI) adsorption, attributed to its redox-active nature. Under optimal conditions (FeCl 3 :lignin:urea = 3:1:0.5), the resulting N-HPC exhibited a high specific surface area (2297.5 m 2 /g), elevated N-5 content (67.08%), and a maximum Cr (VI) adsorption capacity of 627.1   mg/g. Mechanistic studies revealed that reduction–complexation, primarily facilitated by N-5 sites, accounted for up to 87.7% of Cr (VI) removal. The ML-driven inverse design strategy further predicted that precise control of N-5 levels could yield N-HPCs with adsorption capacities exceeding 650   mg/g. This work demonstrates the synergy of ML-guided optimization and mechanistic insight, providing a robust framework for the rational design and accelerated development of sustainable, high-performance adsorbents for heavy metal remediation.

研究领域: 环境科学 · 材料科学 · 化学工程 · 机器学习 · 吸附技术
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CHEMISTRY OF MATERIALS · 2023 · IF 8.6

Copper Tetraselenophosphate Cathode for Rechargeable Magnesium Batteries: A Redox-Active Polyatomic Anion Strategy to Design the Cathode Material

Donggang Tao,Ting Li,Yudi Tang,Yuliang Cao,Fei Xu

Rechargeable magnesium batteries attract interest as advantageous energy-storage devices, but the application is being hampered by the deficiency of suitable cathodes. The traditional method to weaken the interaction between bivalent Mg2+ cations and the cathode material is to increase the anion radius, but excessive expansion of the anion would lead to a decrease of the theoretical capacity and offset the performance improvement. Herein, a new strategy using a redox-active polyatomic anion is developed in terms of copper tetraselenophosphate (Cu3PSe4) fabricated by the PSe43– anion. The covalent P–Se bond facilitates the negative charge delocalization of the PSe43– anion and weakens the interaction with Mg2+ cations, which result in rapid solid-phase Mg2+ diffusion kinetics. The PSe43– anion also provides extra capacities by reversible valence state change of the P element. Cu3PSe4 delivers a high Mg-storage capacity of 225 mAh g–1 at 50 mA g–1 and a superior rate performance of 62 mAh g–1 at 5000 mA g–1, as well as a stable cyclability of 500 cycles. The redox-active polyatomic anion strategy herein opens a new avenue for the exploration of magnesium battery cathodes with a comprehensive consideration of kinetic performance and theoretical capacity.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Energy Storage · 2021 · IF 6.583

Rational design and synthesis of hydrotalcite-like α-Co(OH)2 nanoflakes for extrinsic pseudocapacitive electrodes with superb cycling stability

Weizhi Gong,Mingjun Wang,Yi An,Junli Wang,Liexing Zhou,Yi Xia,Chunjian Wang,Kun Dong,Cheng Pan,Rongfeng Zhou

Cycling stability and specific capacitance are two of important performance parameters for pseudocapacitive electrodes under frequent charging and discharging. Herein, we present a facile solvothermal approach to rationally design and fabricate chiffon-like and hydrotalcite-like α-Co(OH) 2 nanoflakes for extrinsic pseudocapacitive electrode, which exhibits linear galvanostatic discharge behavior and superior charge-storage performance, including high capacitance of 475 F g −1 at 1 A g −1 , excellent rate capability and superb cycling stability with capacitance retention of 93.9% after 10000 cycles at 10 A g −1 . The superior performance is mostly attributed to the good electrical conductivity and stable microstructure of the hydrotalcite-like α-Co(OH) 2 nanoflakes and the abundant redox active sites on the chiffon-like nanoflakes with short and facile electron transport. In addition, other α-Co(OH) 2 samples with different morphologies and size as contrast are prepared and discussed, indicating that the morphology/size design and optimization of the α-Co(OH) 2 could greatly improve the electrochemical energy-storage performance. The findings demonstrate that the chiffon-like and hydrotalcite-like α-Co(OH) 2 nanoflakes have a great practical application potential in long-life and high-performance supercapacitors . This study also presents a facile way to design and prepare nanoflake-like materials with adjustable lateral size and thickness from spherical morphology consisting of nanoflakes.

研究领域: 材料科学 · 电化学 · 纳米技术 · 能源存储
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2022 · IF 5.999

Redox-activity of polydopamine for ultrafast preparation of self-healing and adhesive hydrogels

Lulu Du,Rixin Liao,Huijuan Zhang,Xiongwei Qu,Xiuli Hu

The high adhesive property of polydopamine (PDA) has spurred various hydrogels for biological and medical applications. Herein, a dual-catalytic redox system was constructed by using the inner dynamic redox-activity of PDA and free radical initiator ammonium persulfate (APS) to initiate the polymerization of acrylic acid (AA) monomer to obtain Fe-PDA hydrogels within 2 h at room temperature . Fe-PDA NPs functions as both initiator to activate APS to generate free radicals and promotes the formation of the hydrogel and dynamic cross-linking mediator between the polymer chains. The tensile strength and ductility of the obtained hydrogels vary with the content of Fe-PDA NPs. Hydrogel with 0.15 wt% of Fe-PDA NPs has the highest tensile strength (~0.62 MPa) and hydrogel with 0.6 wt% of Fe-PDA NPs has the highest elongation, about ~650%. The introduction of PDA NPs imparts PAA hydrogel with reproducible adhesive properties and self-healing ability. The doped iron ion further endows hydrogel enhanced photothermal properties (up to 160 ℃ with 808 nm laser irradiation for 120 s) and conductivity .

研究领域: 材料科学 · 生物医学工程 · 化学
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