ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Miao Kan,Xufang Qian,Taiyang Zhang,Dongting Yue,Yixin Zhao
Here we report a highly active electrochemical water splitting electrode fabricated from colloidal IrOx nanoparticles and nanoporous Si stabilized by conformal TiO2. The colloidal amorphous IrOx nanoparticles are highly active for oxygen evolution reaction. However, their application for water splitting has a dilemma that the traditional annealing process could lead to low activities but the nanoparticles based electrode without annealing usually exhibited low stability. This nanostructured water splitting electrode exhibited both the high activities as the colloidal IrOx nanoparticles and comparable stability as a traditional thermal annealing fabricated electrode. The impedance study revealed that conformal TiO2 significantly inhibits the interface oxidation and maintains the high activity of colloidal IrOx nanoparticles catalysts. The conformal TiO2 interface engineering combined with nanocatalysts would be a promising strategy to achieve balanced activities and stability for water splitting.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Ning Zhang,Jiayi Du,Na Zhou,Depeng Wang,Di Bao,Haixia Zhong,Xinbo Zhang
Proton-exchange membrane water electrolysis, particularly driven by renewable electricity, is a sustainable strategy for green hydrogen production . However, developing highly active and stable electrocatalysts to accelerate the oxygen evolution reaction (OER) remains challenging. Herein, we introduce an effective strategy for constructing high-valence metal-doped IrO x with abundant oxygen vacancies, while simultaneously enhancing the catalytic activity and stability of the acidic OER. The synthesized Ta-doped IrO x (350-Ta@IrO x ) exhibits ultramicroscopic nanoparticle morphology and abundant surface oxygen vacancies, enabling a rapid OER process with a low overpotential of 223 mV at 10 mA cm -2 and 147.7 times higher mass activity (1207.4 A g Ir −1 ) than that of commercial IrO 2 at 1.55 V versus the reversible hydrogen electrode. More importantly, 350-Ta@IrO x affords excellent stability with insignificant potential degradation after 500 h of electrolysis at 10 mA cm 2 , originating from the low operating potential and suppressed dissolution and oxidation of oxygen vacancy active sites via Ta doping. Density functional theory calculations suggest that Ta doping and oxygen defect engineering are effective in facilitating the nucleophilic attack of water molecules, thereby accelerating the rate-determining step toward high catalytic OER activity on Ta-doped IrO x . We anticipate that this study will provide an effective method to obtain active and stable electrocatalysts via high-valence metal doping.
研究领域:
化学
·
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 6
·2505-2514
·
IF 2.7
Zeyu Guan,Yuxiao Weng,Jiankun Li,Shiyi Li,Keyu Wang,Linfeng Lei,Yixing Wang,Linzhou Zhuang,Zhi Xu
Proton exchange membrane water electrolysis (PEMWE) can be coupled with renewable energy power generation technology and is considered to be a highly promising hydrogen production technology. However, the acidic electrolyte environment, as well as the numerous sulfonic acid groups on the proton exchange membrane surface, can seriously corrode the oxygen evolution reaction (OER) catalyst and even cause deactivation. To develop an efficient acidic OER catalyst, the IrOx/WO3 heterostructure OER catalyst was prepared by a hydrothermal-calcination method. The coordination environment of IrOx was regulated through the electronic rearrangement effect, improving the OER activity and stability of the catalyst in acidic media. The prepared IrOx/WO3 exhibits excellent OER activity in 0.5 M H2SO4, with an overpotential of only 260 mV to achieve a current density of 10 mA cm−2 and a mass activity of 176.8 A gIr−1. It can stably operate for over 12 hours at a current density of j = 10 mA cm−2.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Xiaoyue Wan,Qi Zhang,Mingming Zhu,Yi Zhao,Yongmei Liu,Chunmei Zhou,Yanhui Yang,Yong Cao
Site-selective deoxygenation of hydroxyl groups represents essential processes to access valuable functionalized bio-based compounds with industrial potential. One of the challenging tasks in this context is to convert biodiesel-derived glycerol in the presence of abundant water directly to 1,3-propanediol (1,3-PDO), a key component of the emerging polymer industry. Herein, a monometallic iridium supported on H-ZSM-5 in the absence of Re oxophilic metal oxides was prepared via grinding-assisted impregnation procedures and attempted as an effective and recyclable catalyst for the aqueous-phase selective hydrogenolysis of glycerol toward 1,3-PDO in the absence of acid additives. The results revealed the necessity to control the Ir domain dispersions, Ir 0 /Ir 3+ ratio and the amounts of overall acid/Brönsted acid sites. Activity depended linearly on the amount of overall and Brönsted acid sites, and 1,3-PDO selectivity increased in the presence of Ir-induced Brönsted acid sites, denoted as Ir-O(H)-H-ZSM-5. We speculate that Ir-O(H)-H-ZSM-5 are generated by the interfacial synergistic interaction between IrO x and H-ZSM-5 through hydrogen spillover and reverse hydrogen spillover according to the reported literatures. The reaction mechanism to elucidate the role of Ir-O(H)-H-ZSM-5 sites in glycerol hydrogenolysis was also postulated based on extensive characterization and catalytic reaction results.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Yunwen Shen,Zhentao Sun,Pei Hu,Wei-Jun Cai,Yiwen Pan
High concentrations of redox substances in the solution may cause severe electrode potential drift, resulting in the inaccuracy of in situ measurements . Sulfide anion , a highly reductive substance, is the killer of all metal oxide electrodes because of its small size and strong surface activity. We first proposed to use SPEEK (SP) with silica-stabilized imidazole-type ionic liquid (ImIL) to fabricate a composite film (SP/SiO x /ImIL) to achieve a high anti-interference ability for metal electrodes. The composite film was especially designed to address the interference caused by sulfide anions and other small-sized anions ( i.e., I − , F − and ascorbic acid). The reduced proton conductivity was restored by introducing ImIL into SPEEK matrix. Open circuit potential tests showed that the potential of the SP/SiO x /ImIL modified IrO x electrode fluctuated within 0.3 mV in 30 min continuous test at a concentration of 10 −3 M Na 2 S, exhibiting good stability in moderately high sulfide solution. It also exhibited fast response and good reversibility. In addition, no potential drift was measured under other anions interferences. XPS survey verified that the Ir 4+ /Ir 3+ ratio of the IrO x electrode did not change before and after application in sulfide-containing solution, indicating that the SP/SiO x /ImIL composite film has good anion isolation capacity.
研究领域:
材料科学
·
电化学
·
环境监测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Li Yanxun,Huang Bo,Zhang Xuning,Ding Jianwei,Zhang Yingyu,Xiao Linge,Wang Boxin,Cheng Qian,Huang Gaosheng,Zhang Hong,Yang Yingguo,Qi Xiaoying,Zheng Qiang,Zhang Yuan,Qiu Xiaohui,Liang Minghui,Zhou Huiqiong
The stability of organic solar cells is a key issue to promote practical applications. Herein, we demonstrate that the device performance of organic solar cells is enhanced by an Ir/IrO x electron-transporting layer, benefiting from its suitable work function and heterogeneous distribution of surface energy in nanoscale. Notably, the champion Ir/IrO x -based devices exhibit superior stabilities under shelf storing ( T 80 = 56696 h), thermal aging ( T 70 = 13920 h), and maximum power point tracking ( T 80 = 1058 h), compared to the ZnO-based devices. It can be attributed to the stable morphology of photoactive layer resulting from the optimized molecular distribution of the donor and acceptor and the absence of photocatalysis in the Ir/IrO x -based devices, which helps to maintain the improved charge extraction and inhibited charge recombination in the aged devices. This work provides a reliable and efficient electron-transporting material toward stable organic solar cells.
研究领域:
材料科学
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能源技术
·
物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Qi Wang,Kaini Zhang,Zhengqi Zhang,Xin Chen,Hao Deng,Weibo Hua,Jinjia Wei,Shaohua Shen,Jie Chen
Reducing iridium (Ir) loading while maintaining efficiency and stability is crucial for the acidic oxygen evolution reaction (OER). In this study, we develop a synthetic method of sequential electrochemical deposition and high-temperature thermal shock to produce an IrOx/Ir-WO3 electrocatalyst with ∼1.75 nm IrOx nanoparticles anchoring on Ir-doped WO3 nanosheets. The IrOx/Ir-WO3 electrocatalyst with a low Ir loading of 0.035 mg cm–2 demonstrates a low overpotential of 239 mV to achieve a current density of 10 mA cm–2 and a mass activity of 6.6 × 104 A gIr–1 @1.75 V vs RHE in 0.5 M H2SO4. IrOx/Ir-WO3 on carbon paper as the anode and Pt/C as the cathode work stably for 40 h at 30 mA cm–2 in a proton exchange membrane water electrolyzer. It is found that the cooperation of lattice-doped Ir and surface-anchored IrOx enhances the activity and stability of IrOx/Ir-WO3 for acidic OER. Specifically, the doped Ir reduces the electron density of the anchored IrOx, thus optimizing the adsorption energy of oxygen-containing intermediates and the kinetic barrier of H2O dissociation, leading to an enhanced activity of IrOx/Ir-WO3. Also, the Ir-WO3 support provides electrons to retard the overoxidation and dissolution of Ir atoms from the anchored IrOx during acidic OER.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers in Energy
·
2022
·Vol. 16
·期 5
·852-861
·
IF 2.964
Li Yonghuan,Song Wei,Jiang Guang,Yang Yue,Yu Hongmei,Shao Zhigang,Duan Fangwei,Yang Yingxuan
Fuel starvation can occur and cause damage to the cell when proton exchange membrane fuel cells operate under complex working conditions. In this case, carbon corrosion occurs. Oxygen evolution reaction (OER) catalysts can alleviate carbon corrosion by introducing water electrolysis at a lower potential at the anode in fuel shortage. The mixture of hydrogen oxidation reaction (HOR) and unsupported OER catalyst not only reduces the electrolysis efficiency, but also influences the initial performance of the fuel cell. Herein, Ti 4 O 7 supported IrO x is synthesized by utilizing the surfactant-assistant method and serves as reversal tolerant components in the anode. When the cell reverse time is less than 100 min, the cell voltage of the MEA added with IrO x /Ti 4 O 7 has almost no attenuation. Besides, the MEA has a longer reversal time (530 min) than IrO x (75 min), showing an excellent reversal tolerance. The results of electron microscopy spectroscopy show that IrO x particles have a good dispersity on the surface of Ti 4 O 7 and IrO x /Ti 4 O 7 particles are uniformly dispersed on the anode catalytic layer. After the stability test, the Ti 4 O 7 support has little decay, demonstrating a high electrochemical stability. IrO x /Ti 4 O 7 with a high dispersity has a great potential to the application on the reversal tolerance anode of the fuel cell.
研究领域:
电化学
·
能源材料
·
燃料电池
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催化化学
·
电极工程
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Jianhua Liao,Yameng Wang,Ming Chen,Min Wang,Jiantao Fan,Hui Li,Haijiang Wang,Lin Zeng,Tianshou Zhao
The addition of an oxygen evolution electrocatalyst to an anode catalyst layer is demonstrated as a practical approach to address the voltage reversal of proton exchange membrane fuel cells (PEMFCs). In this work, IrOX nanoparticles uniformly deposited on niobium-doped TiO2 (IrOX/Nb0.1Ti0.9O2) by a sol–gel method are employed as reversal tolerant anodes (RTAs) for PEMFCs. The membrane electrode assembly (MEA) with this RTA possesses a reversal tolerance time of 29.1 min, which is the best result among all the as-prepared MEAs. Meanwhile, the decrease in the cell voltage of this MEA after reversal testing is only 61 mV at a current density of 1.2 A cm–2 with a degradation rate of 11.1%. The improved reversal tolerance is attributed, in part, to the uniformly distributed IrOX nanoparticles, boosting the oxygen evolution reaction and, in part, to avoid the carbon oxidation reaction by the application of a noncarbon support. This result can lay a fundamental basis for the application of RTA based on a noncarbon support to improve the anode reversal tolerance for PEMFCs.
研究领域:
材料科学
·
能源技术
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 5
·2619-2625
·
IF 3.925
Xuefeng Wang,Haeseong Jang,Zijian Li,Haisen Li,Guangkai Li,Min Gyu Kim,Xuqiang Ji,Qing Qin,Xien Liu
Promoting the activity of Ir-based nanomaterials for oxygen evolution reaction (OER) in acid media without losing their durability is crucial for reducing overpotentials in energy conversion, such as electrochemical water splitting. Here, a nanocomposite composed of a-IrOx and lanthanum salt (LaCO3OH) was constructed to further improve its OER activity by tuning the electronic structure of a-IrOx, because a-IrOx is a well-known critical material as the active layer of Ir-based anodic catalysts. The interaction between Ir and La via O atoms as a bridge in the catalyst IrOx/LaCO3OH, verified by X-ray absorption near edge structure spectroscopy, tunes the electronic structure of a-IrOx and thus obviously enhances its activity for the OER in acid media, compared with commercially available IrO2 as well as most of the reported Ir-based OER electrocatalysts. The overpotential of IrOx/LaCO3OH at a current density of 10 mA cm−2 is 255 mV with a Tafel slope of 55 mV dec−1. This work reveals that the strong electronic interaction between Ir- and La-based materials can efficiently improve activity and reduce energy consumption, as well as enlarging the family of acidic OER electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
Advanced Composites and Hybrid Materials
·
2024
·Vol. 7
·期 2
·1-13
·
IF 23.2
Zhang Hao,Zhu Liyan,Shen Yuhan,Wu Mingjuan,Tian Tian,Tang Haolin
Slow oxygen evolution reaction (OER) and material transport impedance in catalyst-coated membrane (CCM) are major challenges for the practical proton exchange membrane water electrolyzer (PEMWE). Herein, we present a novel OER catalyst by polyether-derived composite oxide pyrolysis with a multilevel porous support and abundant oxygen vacancies to boost efficiency and durability in water electrolysis. The formation of a heterointerface with abundant oxygen vacancies in IrO x improves the catalytic activity and prevents IrO x from peroxidation. Furthermore, the unique pore structure of the support facilitates the mass transport of the anode catalyst layer during water electrolysis at high current density, and the mass transport resistance of the water electrolyzer is only 0.0154 Ω cm 2 at 1.5 A cm −2 . When used in a PEMWE, the prepared electrocatalysts have an impressive electrochemical performance of 1.87 V at 3·A cm −2 with an Ir loading of only 0.91 mg cm −2 . This approach highlights the importance of oxygen vacancies and transportation in the catalyst-support interface, providing a promising solution for high-rate practical water electrolysis. Graphical
Efficient OER supported catalysts enriched with oxygen vacancies for PEMWE applications
研究领域:
电化学
·
催化
·
材料科学
·
能量转换
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Yuanyi xiang,Haiwen Qiu,Yuqing Huang,Qinghong Huang,Xiaoyan Luo,Zhou Yi,Yuping Wu
Proton exchange membrane (PEM) water electrolysis has broad application prospects for clean hydrogen production owing to its high efficiency, compact structure, rapid response, and flexible load regulation. However, the sluggish kinetics of the oxygen evolution reaction (OER) under strongly acidic conditions still poses a major challenge to the development of efficient and stable acidic OER electrocatalysts. In this work, a low-crystallinity IrO x /Ir catalyst with a gradient-distributed IrO x coating was successfully prepared by a hydrothermal method. In acidic OER tests, the catalyst exhibited excellent electrocatalytic performance, delivering a mass activity 218 times higher than that of commercial IrO 2 at 1.55 V vs. RHE, and requiring an overpotential of only 231 mV to reach 10 mA·cm −2 . The incorporation of non-crystalline metallic Ir 0 significantly improves the electrical conductivity and intrinsic catalytic activity of the catalyst. Meanwhile, the outer layer of more crystalline iridium oxide effectively protects the highly active low-crystallinity iridium oxide in the interior from dissolution and corrosion, so that the catalyst shows no obvious activity decay after 300 h of continuous operation, indicating good stability.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）