WATER RESEARCH
·
2019
·
IF 7.913
Dongni Sun,Xiaoting Hong,Keming Wu,K.S. Hui,Yingying Du,K.N. Hui
Electro-oxidation using RuO 2 –IrO 2 /Ti plate anode and electrocoagulation using iron plate anode were widely applied to remove ammonia and phosphate in an aquatic environment, respectively. In this work, we designed magnetically bound ZVI microparticles on RuO 2 –IrO 2 /Ti plate as a composite electrode for the simultaneous removal of ammonia and phosphate from aqueous solution via combined EO and EC (EO/EC) processes. We present a series of experiments to study such simultaneous removal under an electric field via the EO/EC process. In the electrochemical unit, mZVI-RuO 2 -IrO 2 /Ti, mZVI-graphite, and RuO 2 –IrO 2 /Ti electrodes were used as anodes. The influence of applied voltage, initial pH, zero-valent iron dosage, reaction temperature, and organic compounds on the EO/EC process was also examined. Ammonia and phosphate could be completely removed at an applied voltage of 10 V, pH of 7, zero-valent iron dosage of 0.1 g, and reaction temperature of 35 °C using mZVI-RuO 2 -IrO 2 /Ti anode when influent ammonia and phosphate concentrations is 200 and 100 mg L −1 . Ammonia degradation was consistent with pseudo-zero-order kinetic model. The characterization was analyzed by scanning electron microscope-energy dispersive spectrometer (SEM-EDS), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Hence, the mZVI-RuO 2 -IrO 2 /Ti electrode can be used for efficient simultaneous removal of ammonia and phosphate.
研究领域:
环境科学
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电化学工程
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xiaoqin Li,Yuqi Su,Ronghai Bai,Qibin Li
Electrochemical oxidation (EO) effectively degrades phenolic compounds in phenol-containing wastewater, but the chlorinated byproducts generated during the process raised concerns. In this study, degradation efficiency of phenol and formation rules of chlorinated byproducts in the presence of chlorine (Cl − )were systematically and comparatively studied in two EO systems with boron-doped diamond (BDD) and ruthenium-iridium-coated titanium (RuO 2 -IrO 2 /Ti) as anodes. The results showed that Cl − significantly enhanced phenol degradation efficiency of the two anode systems. At the same Cl − concentration, degradation efficiency of BDD-EO was superior to that of RuO 2 -IrO 2 /Ti-EO, it had a higher apparent removal rate for phenolic compounds, including phenol, 4-NP, 4-CP, BPA, and RES, and was less affected by coexisting ions. However, in the BDD-EO system, the total amount of produced chlorinated byproducts (3.593 mM Cl) was approximately 50 times greater than that produced in the RuO 2 -IrO 2 /Ti-EO system (0.0723 mM Cl). These chlorinated byproducts included inorganic chloro-byproducts (ClO 3 − and ClO 4 − ) and organic chloro-byproducts (such as chloroform, trichloroacetic acid, and trichloroacetaldehyde). The results confirmed that HOCl generated by the oxidation of Cl − on BDD and RuO 2 -IrO 2 /Ti anodes through the • OH/direct electron transfer was the key active species for enhancing the phenol degradation and driving the formation of chlorinated byproducts. The toxicity assessment shows that the additive toxicity of inorganic chloro-byproducts in the RuO 2 -IrO 2 /Ti-EO system is approximately 1/57 that in the BDD-EO system, and the toxicity of organic chloro-byproducts is approximately 1/18. Selecting the appropriate anode is therefore critical to balance treatment efficiency with the need to minimize toxic chlorinated byproducts.
研究领域:
环境工程
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电化学
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水处理技术
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化学毒理学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
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IF 5.31
Anlin Xu,Weiqing Han,Jiansheng Li,Xiuyun Sun,Jinyou Shen,Lianjun Wang
A novel dual tubular membrane electrodes reactor was fabricated to degrade a refractory heterocyclic compound-tricyclazole using a tubular membrane Ti/IrO 2 –Ta 2 O 5 as anode and a carbon black-polytetrafluoroethylene (CB-PTFE) modified graphite membrane as cathode. Field emission scanning electron microscopy (FE-SEM), cyclic voltammetry (CV), Linear Sweep Voltammetry (LSV) and accelerated lifetime tests revealed that a porous tubular membrane Ti/IrO 2 –Ta 2 O 5 performed better electrocatalytic activity and high stability under acidic conditions. Meanwhile, the effects of aeration on electrogeneration of hydrogen peroxide (H 2 O 2 ) were assessed and the role of anode in dynamic system was elucidated by comparing with the static system. The influence of the operative parameters such as current density (2.5–12.5 A/m 2 ), membrane flux (52–178 L/m 2 ·h) and pH (3–11) were optimized and monitored. It is demonstrated that tubular membrane Ti/IrO 2 –Ta 2 O 5 anode provided enough oxygen to electrogenerate H 2 O 2 , up to 1586 mg/m 2 ·h, at 10 A/m 2 without aeration in acidic solution. Even if no circulation of the influent, the best removal rate of contaminants reached a stable value 79% at 20 min, which was 6.58-fold greater than the sum of the individual electrochemical oxidation. Synergism was observed during the dual tubular membrane E-Fenton system.
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DOI
高影响因子
Water
·
2022
·Vol. 14
·期 7
·1044
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IF 3.53
Miao Deng,Keming Wu,Tao Yang,Deyou Yu,Gaojie Liu,Shuai Gong,Dongni Sun,Michal Petru
The Electro-Fenton (E-Fenton) technique has shown great potential in wastewater treatment, while the sustainable and continuing supply of Fe2+remains challenging. Herein, we demonstrate the construction of a novel E-Fenton system by magnetically decorating zero-valent iron (ZVI) onto a RuO2-IrO2/Ti (ZVI-RuO2-IrO2/Ti) electrode for high-efficient treatment of pharmaceutical wastewater, which is considerably refractory and harmful to conventional biological processes. By using ZVI as a durable source of Fe(II) irons, 78.69% of COD and 76.40% of TOC may be rapidly removed by the developed ZVI-RuO2-IrO2/Ti electrode, while the ZVI-RuO2-IrO2/Ti electrode using ZVI only reduces 35.64% of COD under optimized conditions at initial COD and TOC values of 5500 mg/L and 4300 mg/L, respectively. Moreover, the increase in BOD5/COD from 0.21 to 0.52 highlights the enhanced biodegradability of the treated effluent. The analysis of a simultaneously formed precipitation on electrodes suggests that the coagulation process dominated by Fe3+/Fe2+also plays a non-negligible role in pharmaceutical wastewater treatment. In addition, the monitoring of the evolution of nitrogen elements and the formation of by-products in the E-Fenton process verifies its great capacity toward those organic pollutants found in pharmaceutical wastewater. Our study offers a practical solution for enhancing the performance of E-Fenton systems, and effectively treating refractory pharmaceutical wastewater.Keywords:electro-oxidation;zero-valent iron;pharmaceutical wastewater;E-Fenton process
研究领域:
环境科学
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化学工程
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
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IF 8.4
Liyue Zhang,Qiucheng Xu,Yanjie Hu,Ling Chen,Hao Jiang
Anion exchange membrane water electrolysis (AEMWE) is one of the most promising technologies for producing green hydrogen; however, they still suffer from durability issues. One task is to find suitable electrolyte conditions for anode catalysts that endow them with both high activity and stability. Herein, we benchmark the pH–stability relationship of four typical metal oxides as anode catalysts in the AEMWE. Their electrochemical performance and structural stability were in-depth analyzed through impedance, dissolved composition in the electrolyte, and correlated Pourbaix diagram. NiFe2O4 with the best activity and stability in the strong alkaline (pH = 14) shows terrible stability in pure water, which is then verified due to the severe Fe leaching, and it cannot be alleviated by alkaline pre-activation. Notably, Co3O4 shows comparable activity and stability to IrO2 in pure water and weak alkaline conditions. At pH = 12, it entails only ∼2.18 V to reach 1.0 A cm–2 and stabilizes for 40 h, being superior to others. This work screens out suitable transition metal oxides as a substitute for noble metals and their optimal application scenarios for AEMWE.
研究领域:
电化学
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材料科学
·
可再生能源
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Zuobo Yang,Xiaokuan Wu,Leilei Cai,Jimmy Yun,Jie Zhang,Xin Liang,Hong Zhao
Proton-exchange membrane water electrolysis (PEMWE) holds great promise for hydrogen production applications. However, the reliance of PEMWE membrane electrodes on high loadings of expensive iridium poses a significant barrier to their commercial viability. Therefore, the development of high-performance oxygen evolution catalysts with a low iridium content is of critical importance. In this research, a porous antimony tin oxide (ATO) conductive support with a particle assembly aggregate structure was fabricated by a carbon template removal method. ATO-supported IrO2 exhibits significantly improved oxygen evolution reaction (OER) activity, with a much lower overpotential compared to the unsupported IrO2 catalyst. Moreover, it achieves 1.8 V at 2 A cm–2 with an ultralow loading of iridium (0.3 mgIr cm–2) for the proton-exchange membrane electrolyzer. Characterization techniques and density functional theory calculations have elucidated that the enhanced performance is attributed to the porous morphology of ATO and the strong metal oxide–support interaction between IrO2 and the ATO support. These findings validate the practicality of conductive nanostructured antimony-tin-oxide-supported catalysts for PEMWE applications and offer a pathway for the design of low-Ir OER catalysts.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2019
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IF 7.467
Zhiyu Shao,Jing Sun,Niankun Guo,Feng He,Keke Huang,Fuli Tian,Qin Wang
Designing highly active and low-cost electrocatalysts towards oxygen evolution reaction has ignited much interest in recent years. Thereby, rational design of those catalysts is an urgent topic that must be addressed. Herein, an effective strategy is demonstrated to be beneficial to the formation of hierarchical nitride phosphide hybrid with abundant oxygen vacancies . This hybrid catalyst exhibits an excellent OER catalytic performance, as demonstrated by an ultralow Tafel slope of 41 mV·dec −1 and an overpotential of 290 mV at 10 mA cm −2 in 1.0 M KOH solution, which is superior to those of the pure nitride, phosphide, and the commercial IrO 2 catalysts. The outstanding catalytic performance can be attributed to the specific heterojunction structure, accessible active sites, and abundant oxygen vacancies, which can facilitate the charge transport and the release of the O 2 bubbles. This study not only provides a facile strategy for constructing surface oxygen vacancies onto phosphide/nitride hybrid, but also exhibits an insight into the nature of hierarchical electrocatalyst with multiple active sites.
研究领域:
电化学
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材料科学
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催化
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产品关联
DOI
高影响因子
Aggregate
·
2024
·
IF 13.9
Shuqi Wu,Fang Nan,Kewen Zhang,Wan Hao,Di Shi,Yang Li,Wei Deng,Nur Jarhen,Kaixuan Li,Yunyun Xiao,Jun Li,Xiao Lin
Osteoarthritis (OA) is associated with metabolic imbalance of articular cartilage and an increase of intracellular reactive oxygen species (ROS). Synergistic therapy based on the codelivery of ROS scavengers and antisense oligonucleotides (ASO) into chondrocytes has the potential to effectively treat OA. Here, we developed a novel biocompatible metal-organic framework (MOF)-encapsulated nanozyme/ASO delivery platform (miR/IrO 2 @ZIF-8) for OA treatment. IrO 2 nanoparticles with the catalytic activities of superoxide dismutase/catalase were synthesized using a hydrothermal method, resulting in excellent ROS scavenging performance. IrO 2 was further loaded into zeolitic imidazolate framework-8 (ZIF-8) to maintain its catalytic efficacy and regulate its size, surface charge, and biocompatibility to enhance the therapeutic effect of the platform. As an effective ASO delivery carrier, the synthesized IrO 2 @ZIF-8 exhibited high antagomiR-181a loading and lysosomal escape capacity, enabling it to rebalance cartilage metabolism. In vitro experiments showed that miR/IrO 2 @ZIF-8 could restore ROS levels, mitochondrial membrane potential, and lipid peroxidation in chondrocytes. At the same time, the expression levels of proinflammatory markers (IL-1β, IL-6, and COX-2) as well as the extracellular matrix degrading enzymes (ADAMTS-5 and MMP13) were downregulated, indicating effective antioxidant, anti-inflammatory, and anticartilage degradation effects. Notably, miR/IrO 2 @ZIF-8 was able to deliver IrO 2 nanoparticles and antagomiR-181a to the cartilage tissue at a depth of up to 1.5 mm, thus solving the problems of poor permeability and difficult retention of drugs in cartilage tissue. This further improves the synergistic therapeutic effect on OA by inhibiting cartilage degradation. The combination of MOF-encapsulated IrO 2 nanozymes with antagomiR-181a has an excellent therapeutic effect on OA, offering a promising translational medicine paradigm.
研究领域:
纳米技术
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药学
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生物医学工程
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骨科
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材料科学
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DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Zhu Yiming,Wang Jiaao,Koketsu Toshinari,Kroschel Matthias,Chen Jin-Ming,Hsu Su-Yang,Henkelman Graeme,Hu Zhiwei,Strasser Peter,Ma Jiwei
Designing active and stable electrocatalysts with economic efficiency for acidic oxygen evolution reaction is essential for developing proton exchange membrane water electrolyzers. Herein, we report on a cobalt oxide incorporated with iridium single atoms (Ir-Co 3 O 4 ), prepared by a mechanochemical approach. Operando X-ray absorption spectroscopy reveals that Ir atoms are partially oxidized to active Ir >4+ during the reaction, meanwhile Ir and Co atoms with their bridged electrophilic O ligands acting as active sites, are jointly responsible for the enhanced performance. Theoretical calculations further disclose the isolated Ir atoms can effectively boost the electronic conductivity and optimize the energy barrier. As a result, Ir-Co 3 O 4 exhibits significantly higher mass activity and turnover frequency than those of benchmark IrO 2 in acidic conditions. Moreover, the catalyst preparation can be easily scaled up to gram-level per batch. The present approach highlights the concept of constructing single noble metal atoms incorporated cost-effective metal oxides catalysts for practical applications.
研究领域:
电化学
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材料科学
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催化
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能源存储与转化
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产品关联
DOI
PubMed
高影响因子
Scientific Reports
·
2019
·Vol. 9
·期 1
·1-10
·
IF 4.011
Sun Juan,Zhang Zonghuai,Gong Yansheng,Wang Huanwen,Wang Rui,Zhao Ling,He Beibei
The development of highly active and cost-effective catalysts based on noble metal free oxygen electro-catalysis is critical to energy storage and conversion devices. Herein, we highlight a plasma-treated Bi 0.1 (Ba 0.5 Sr 0.5 ) 0.9 Co 0.8 Fe 0.2 O 3−δ perovskite (denoted as P-Bi 0.1 BSCF) as a promising catalyst for oxygen evolution reaction (OER) in alkaline media. H 2 /Ar plasma engraving could significantly increase electrochemically active O 2 2− /O − concentration and tune the electronic structure of Co ions efficiently, and consequently tailor the intrinsic electrocatalytic ability for OER. Of note, P-Bi 0.1 BSCF, with unique crystalline core/amorphous shell structure, exhibits an enhanced intrinsic OER activity and higher stability than the noble metal IrO 2 catalyst, which outperforms most of the reported perovskite catalysts. The present work provides new insights into exploring efficient catalysts for OER, and it suggests that, in addition to the extensively applied for surface treatment of various catalysts such as carbons and metal oxides, the plasma engraved perovskite materials also exhibits great potential as precious metal-free catalysts.
研究领域:
材料科学
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电化学
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催化
·
能源存储与转换
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Yufeng Qin,Yifan Wang,Rou Wen,Longxiang Wang,Meiling Dou,Feng Wang
The need to use expensive and scarce Ir-based catalysts in the oxygen evolution reaction (OER) hinders the large-scale application of proton exchange membrane water electrolysis (PEMWE). Herein, we present an effective interface-engineering strategy to boost the efficacy of low-Ir catalysis of OER by means of electron transfer and lattice oxygen stabilization at the catalyst–support interface by utilizing a highly conductive (∼960 S cm–1) Ti4O7 support to strongly anchor IrO2 nanoparticles. Experimental and theoretical calculations suggest that Ti4O7 tailors the Ir electronic structure that results from the formation of Ir–O–Ti bonds at the IrO2–Ti4O7 interface, resulting in a lowered d-band center that weakens the adsorption of oxygen intermediates on Ir sites and thus boosts OER catalysis. The Ir–O–Ti bonds formed at the interface stabilize lattice oxygen in IrO2, facilitating a stable lattice oxygen mechanism path for OER catalysis. The interface effect results in superior OER activity with an overpotential of 244 mV at 10 mA cm–2 and a high mass activity of 1342.9 A gIr–1 (93.25× that of commercial IrO2), and the material also shows better durability than commercial IrO2. This interface-engineering strategy affords a strong catalyst–support interaction and should facilitate the design of high-performance catalysts for PEMWE applications.
研究领域:
催化
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材料科学
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电化学
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子