CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Dandan Li,Tan Li,Genyan Hao,Wenjun Guo,Shuai Chen,Guang Liu,Jinping Li,Qiang Zhao
A hybrid oxygen evolution catalyst, IrO 2 @single-layer NiFe layered double hydroxides (SL-NiFe LDHs), is successfully synthesized by anchoring highly dispersed IrO 2 nanoparticles to SL-NiFe LDHs nanosheets with oxygen vacancies. Typically, during the synthesis process, the functional group –NH 2 from the external anchor formamide acts as a coordination site to control the nucleation and growth of nanoparticles , which can ensure high dispersion without aggregation of IrO 2 on SL-NiFe LDHs. In addition, this reducing synthetic environment causes a large number of holes and grooves in the NiFe-LDHs nanosheets, which result in the formation of oxygen vacancies in the SL-NiFe LDHs. The loading of IrO 2 nanoparticles and the formation of oxygen vacancies endow IrO 2 @SL-NiFe LDHs with excellent performance for the oxygen evolution reaction (OER). IrO 2 @SL-NiFe LDHs nanosheets display outstanding OER performance with an overpotential of 270 mV at a current density of 10 mA cm −2 and good stability. Density functional theory (DFT) calculations indicate that the hybridization of IrO 2 and SL-NiFe LDHs accelerates the reaction step. Notably, the Ir sites at the edges are more conducive to the formation of oxygen, and the oxygen sites on SL-NiFe LDHs are more conducive to the cleavage of the O–H bond, thereby improving the OER activity. This work highlights a potential synthetic strategy that can combine nanoprecious metals with transition metals to prepare highly active electrocatalysts for efficient water oxidation reactions.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2020
·
IF 7.246
Bao Liu,Kexuan Lyu,Yongqiang Chen,Baozhong Ma,Chengyan Wang
Manganese electrodeposition experiments were performed in an anion-exchange membrane (AEM) electrolysis reactor using Ti/IrO 2 –RuO 2 –SiO 2 anode. The influence of Mn 2+ concentration, cathode current density (CCD), (NH 4 ) 2 SO 4 concentration, SeO 2 concentration and electrolysis time on the cell voltage (CV), cathode current efficiency (CE) and specific energy consumption (SEC) of manganese electrodeposition was investigated. The crystalline structure, chemical composition and morphology of the deposited manganese metal and the generated dark mass were analyzed using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FESEM) and energy dispersive spectroscopy (EDS) measurements. The obtained results reveal that the crystalline structure of the deposited manganese metal was α-Mn. The dark mass of MnOOH would be generated and precipitated on the surface of the cathode, inhibiting the electrodeposition of manganese metal when the operating condition was not well controlled. Considering the CE, SEC and environmental aspect, the operating condition of Mn 2+ concentration = 30 g L −1 , CCD = 350 A m −2 , (NH 4 ) 2 SO 4 concentration = 110 g L −1 and SeO 2 concentration = 0.03 g L −1 was regarded as the best condition for manganese electrodeposition. Under this condition, the CE was 78.3% and the SEC was 4346–4433 kW h t −1 after electrolyzing for 24 h. Compared with the traditional approach, the CE increased by about 10% and the SEC decreased by about 27%. In addition, the electrolytic manganese anode slime was not generated during the manganese electrodeposition process . This approach is recommended as it will reduce the energy consumption and the quantities of solid waste discharge of manganese electrodeposition.
研究领域:
材料科学
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电化学工程
✓ 已验证
DOI
高影响因子
Journal of Water Process Engineering
·
2023
·
IF 7
Hao Li,Jiahao Zhang,Yiqi Du,Meixia Shi,Xinmou Kuang,Xiaolan Shen,Wenting Si
Electrochemical activation of persulfate is an efficient and green technology. In this study, the differences in the pollutant degradation efficiency and peroxydisulfate (PDS) activation mechanism were compared via electrochemical activation of PDS using only an IrO 2 anode, an IrO 2 cathode, and both an IrO 2 anode and stainless steel (SS) cathode. In these methods, the degradation of acid orange (AO) 74 conformed to the pseudo-first-order kinetic degradation model. The electrochemical activation of PDS using an IrO 2 anode resulted in the highest AO 74 degradation efficiency of 81.7 % with a degradation rate constant of 0.58 h −1 . The results of radical quenching and cyclic voltammetry indicated that during the electrochemical activation of PDS using an IrO 2 anode, direct electron transfer and nonradical oxidation contributed to AO 74 degradation. Using an IrO 2 cathode, the contribution to AO 74 degradation was mainly OH, while using an IrO 2 anode and SS cathode, the contribution was the joint action of the nonradical and radical oxidation. Furthermore, during the electrochemical activation of PDS using an IrO 2 anode, the degradation rate exhibited a good linear relationship with the current density and PDS concentration. The addition of Cl − considerably enhanced AO 74 degradation.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Qian Gao,Saren Ao,Hui Chen,Xiaoxin Zou,Cundi Wei,Guo-Dong Li
IrO 2 -loaded porous foam-like Ga 1.4 In 0.6 O 3 nanofibers with ultrathin pore walls were synthesized via a simple electrospinning and impregnation method for the detection of formaldehyde. This gas sensor based on IrO 2 -loaded Ga 1.4 In 0.6 O 3 nanofibers showed excellent sensitivity and selectivity towards trace formaldehyde. Especially, the response of the gas sensor based on 1% IrO 2 -Ga 1.4 In 0.6 O 3 nanofibers is as high as 46 towards 10 ppm formaldehyde, while it is only 7 for the gas sensor based on Ga 1.4 In 0.6 O 3 . Moreover, the gas sensor based on 1% IrO 2 -Ga 1.4 In 0.6 O 3 exhibited remarkable selectivity towards formaldehyde. The high sensitivity and good selectivity of IrO 2 -loaded porous Ga 1.4 In 0.6 O 3 nanofibers could be attributed to the specific catalytic activity of IrO 2 , the unique composition and the ultrathin structure of Ga 1.4 In 0.6 O 3 .
研究领域:
材料科学
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纳米技术
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环境监测
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 9
·3579-3588
·
IF 8.307
Jianjun Zhou,Tian Wang,Cheng Cheng,Fan Pan,Yunqing Zhu,Hongrui Ma,Junfeng Niu
Electrocatalytic oxidation is regarded as an effective technique for decomposing refractory organic compounds like perfluorooctanoic acid (PFOA). However, achieving highly efficient and long-life electrodes is still a great challenge. Herein, Ti/RuO2–IrO2@Pt anodes consisting of Pt4+ and Pt0 species were fabricated by combining modified microemulsion technology with a calcination process, in which Pt nanoparticles were highly dispersed and encapsulated in Ru–Ir composite oxides to form a strong metal–support interaction (SMSI) structure. The as-constructed SMSI layer on the Ti/RuO2–IrO2@Pt anode resulted in the improvement of the charge transfer capability and also increased the degradation (99.30%) and mineralization (91.32%) of PFOA during the electrochemical oxidation process. Notably, the service lifetime of Ti/RuO2–IrO2@Pt anodes was remarkably improved from 24 to 42.3 h compared to commercial Ti/RuO2–IrO2 anodes. Moreover, the possible degradation mechanism of PFOA was also speculated through the detection of short-chain perfluorocarboxylic acids and reactive radicals. These results not only revealed that the concept and methodology of SMSI could be an effective way for constructing highly efficient and stable electrocatalysts but also greatly advanced fundamental understanding.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Hanyang Li,Yuexin Xu,Ning Lv,Qiuyitong Zhang,Xiaolian Zhang,Zijie Wei,Yadong Wang,Haolin Tang,Hongfei Pan
The development of polymer electrolyte membrane electrolysis of water is mainly limited by the high cost of noble metals and inadequate stability owing to the slow reaction kinetics of the oxygen evolution reaction and the restrictions of strongly acidic operating environments. To improve the utilization of noble metals, we use Ti-doped SnO2 as a carrier to support active species IrO2. The results show that the introduction of Ti element can inhibit the grain growth and help to improve the electrical conductivity of SnO2. Electrochemical tests for the catalysts show that 40 wt % IrO2/TSO has the best mass-normalized charge (231.24 C g–1 IrO2) and current density (714.85 A g–1 IrO2) at 1.6 V with the overpotential of only 271 mV at 10 mA cm–2, which is attributed to the outstanding dispersion effect of Ti-doped SnO2 and the synergy between the active species and the introduction of Ti element. The comprehensive advantages exhibited by the Ti-doped SnO2 support provide an alternative solution to reduce the cost of noble metal catalysts by improving the catalytic activity and stability.
研究领域:
电化学
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材料科学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 22
·8047-8055
·
IF 6.482
Sen Wang,Hong Lv,Songhu Bi,Tianqi Li,Yongwen Sun,Wenxuan Ji,Cong Feng,Cunman Zhang
Developing cost-effective Ir-based anode catalysts for proton exchange membrane (PEM) water electrolysis has been recognized as an efficient and pragmatic approach; however, many challenges remain to lower the Ir content while maintaining high electrocatalytic performance. Herein, an effective strategy of tailoring IrO2@TiN1+x nano-heterojunctions by defects is reported, aiming at enhancing the intrinsic oxygen evolution reaction (OER) activity of IrO2 at a low Ir amount. A remarkable OER activity in an acidic solution is achieved for IrO2@TiN1+x with 7.3 times of mass activity and 1.8 times of specific activity relative to IrO2. As the anode electrode in a PEM single cell, IrO2@TiN1+x also reveals the optimal activity with 1.916 V at 2 A cm−2, which is 57 mV and 130 mV lower than that of IrO2@TiN and IrO2, respectively. Meantime, the IrO2@TiN1+x electrode manifests good stability at 1 A cm−2 for 100 h. Electrochemical characterization analysis and DFT calculation results indicate that the increase in the number of active sites and the modulating electronic interaction between IrO2 and TiN1+x could multiply the active sites and accelerate the OER kinetics of IrO2. Thus, the IrO2@TiN1+x nano-heterostructure reveals superior electrocatalytic performance and good stability at a low Ir content.
研究领域:
材料科学
·
电化学
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yixi Wang,Wenqing Xu,Chaoqun Li,Yang Yang,Zanbu Geng,Tingyu Zhu
Gaseous ammonia (NH 3 ), especially that emitted from selective catalytic reduction with NH 3 (NH 3 –SCR) units in the atmosphere is potentially harmful to both human health and the environment. The noble metal catalytic oxidation technology placed behind the SCR unit has been considered to be a promising method for decreasing NH 3 slip. In this study, we prepared Ir/Al 2 O 3 catalysts using two different crystal structures of Al 2 O 3 (α–Al 2 O 3 or γ–Al 2 O 3 ) as supported by an impregnation method and evaluated the performance of the selective catalytic oxidation of NH 3 (NH 3 –SCO). We found that the Ir/γ–Al 2 O 3 catalyst performed better than the Ir/α–Al 2 O 3 catalysts, with 99% of NH 3 converted at 260 °C. The X–ray absorption fine structure revealed that the active species on the Ir/Al 2 O 3 catalysts are mainly oxidized IrO 2 . High–angle annular dark–field images of aberration–corrected scanning transmission electron microscopy revealed that IrO 2 species over 1 nm in diameter are beneficial for activity. In situ diffuse reflectance for infrared Fourier transform spectroscopy studies suggested that the differences in NH 3 –SCO activity were caused by the activity of reactive oxygen species, and the formation of –NH 2 may be the decisive step of the NH 3 oxidation reaction.
研究领域:
催化
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Chenglong Ma,Wei Sun,Waqas Qamar Zaman,Zhenhua Zhou,Hao Zhang,Qicheng Shen,Limei Cao,Ji Yang
Research has been focused on regulating the amorphous surface of Ir-based materials to achieve a higher oxygen evolution reaction (OER) activity. The IrOx amorphous layer is generally considered to be substantial enough to break the limitation created by the conventional adsorbate evolution mechanism (AEM) in acidic media. In this work, we used lanthanides to regulate IrOx amorphization–crystallization through inhibiting the crystallization of iridium atoms in the calcination process. The chosen route created abundant crystalline–amorphous (c-a) interfaces, which greatly enhanced the charge transfer kinetics and the stability of the materials. The mass activity of iridium in the synthesized IrO2@LuIr1–nOx(OH)y structure reached 128.3 A/gIr, which is 14.6-fold that of the benchmark IrO2. All the IrO2@LnIr1–nOx(OH)y (Ln = La–Lu) structures reflected 290–300 mV of overpotential at 10 mA/cmgeo2. We demonstrate that a highly active c-a interface possesses an efficient charge transfer capability and is conducive to the stability of the activated oxygen species. The surface-activated oxygen species and the tensile strain [IrO6] octahedron regulated by lanthanides are synergistically beneficial for increasing the intrinsic OER activity. Our research findings introduce c-a interface generation by the regulation of lanthanides as a new method for the rational design of robust OER catalysts.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 14
·143503
·
IF 3.721
Yijie Liu,Xianzhe Meng,Chao Li,Yifan Gong,Juan Wang,Jiang Bo
Non-biodegradable pharmaceuticals are a group of emerging contaminants that have gained much attention because of their potential risk of inducing adverse ecological and health effects. An efficient Ti/SnO2-Sb2O5-IrO2-RuO2 electrode was prepared by Pechini method and employed as the anode for electrochemical degradation of selected pharmaceuticals (i.e., ibuprofen, atenolol, and carbamazepine). Compared its counterparts, Ti/SnO2-Sb2O5-IrO2-RuO2 exhibited higher oxygen evolution potential, lower chlorine evolution potential, larger active area, and higher stability. Unlike the negligible effect of solution pH from 4.0 to 10.0, increasing current density favored the target pollutants and COD removal. The removal of IBU was mainly attributed to the reaction with •OH, the contribution of which to IBU removal was enhanced with increasing current density. In contrast to IBU, the removal of ATEN and CBZ was mainly ascribed to the reaction with selective radical chlorine species (RCS) mainly in the form of Cl•, which was produced from direct oxidation of Cl− or indirect oxidation by •OH. It was found that the removal of ATEN and CBZ was less affected by dissolved organic matter (DOM) than that of IBU in municipal effluent. This study demonstrates that Ti/SnO2-Sb-RuO2-IrO2 is an attractive electrode for the destruction of pharmaceutical contaminants.
研究领域:
环境科学
·
电化学工程
·
污染控制
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 5
·2189
·
IF 4.6
Yunqing Zhu,Bingqing Li,Yongming Wang,Tian Wang
Electrocatalytic oxidation (ECO) has attracted attention because of its high efficiency and environmental friendliness in water treatment. The preparation of anodes with high catalytic activity and long service lifetimes is a core part of electrocatalytic oxidation technology. Here, porous Ti/RuO2-IrO2@Pt, Ti/RuO2-TiO2@Pt, and Ti/Y2O3-RuO2-TiO2@Pt anodes were fabricated by means of modified micro-emulsion and vacuum impregnation methods with high porosity titanium plates as substrates. The scanning electron microscopy (SEM) images showed that RuO2-IrO2@Pt, RuO2-TiO2@Pt, and Y2O3-RuO2-TiO2@Pt nanoparticles were coated on the inner surface of the as-prepared anodes to form the active layer. Electrochemical analysis revealed that the high porosity substrate could result in a large electrochemically active area, and a long service life (60 h at 2 A cm−2current density, 1 mol L−1H2SO4as the electrolyte, and 40 °C). The degradation experiments conducted on tetracycline hydrochloride (TC) showed that the porous Ti/Y2O3-RuO2-TiO2@Pt had the highest degradation efficiency for tetracycline, reaching 100% removal in 10 min with the lowest energy consumption of 167 kWh kg−1TOC. The reaction was consistent with the pseudo-primary kinetics results with a k value of 0.5480 mol L−1s−1, which was 16 times higher than that of the commercial Ti/RuO2-IrO2electrode. The fluorospectrophotometry studies verified that the degradation and mineralization of tetracycline were mainly ascribed to the •OH generated in the electrocatalytic oxidation process. This study thus presents a series of alternative anodes for future industrial wastewater treatment.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2024
·
IF 14.3
Yuhan Shen,Shengqiu Zhao,Fanglin Wu,Hao Zhang,Liyan Zhu,Mingjuan Wu,Tian Tian,Haolin Tang
Acidic seawater electrolysis offers significant advantages in high efficiency and sustainable hydrogen production. However, in situ electrolysis of acidic seawater remains a challenge. Herein, a stable and efficient catalyst (SPTTPAB/IrO 2 ) is developed by coating iridium oxide (IrO 2 ) with a microporous conjugated organic framework functionalized with sulfonate groups (-SO 3 H) to tackle these challenges. The SPTTPAB/IrO 2 presents a -SO 3 H concentration of 5.62 × 10 −4 mol g −1 and micropore below 2 nm numbering 1.026 × 10 16 g −1 . Molecular dynamics simulations demonstrate that the conjugated organic framework blocked 98.62% of Cl − in seawater from reaching the catalyst. This structure combines electron conductivity from the organic framework and proton conductivity from -SO 3 H, weakens the Cl − adsorption, and suppresses metal-chlorine coupling, thus enhancing the catalytic activity and selectivity. As a result, the overpotential for the oxygen evolution reaction (OER) is only 283 mV@10 mA cm −2 , with a Tafel slope of 16.33 mV dec −1 , which reduces 13.8% and 37.8% compared to commercial IrO 2 , respectively. Impressively, SPTTPAB/IrO 2 exhibits outstanding seawater electrolysis performance, with a 35.3% improvement over IrO 2 to 69 mA cm −2 @1.9 V, while the degradation rate (0.018 mA h −1 ) is only 24.6% of IrO 2 . This study offers an innovative solution for designing high-performance seawater electrolysis electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 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）