Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Quan Quan,Zhang Yuxuan,Li Haifan,Wang Wei,Xie Pengshan,Chen Dong,Wang Weijun,Meng You,Yin Di,Li Yezhan,Song Dongyuan,Chen Lijie,Li Shaohai,Yang Cheng,Yanagida Takeshi,Wong Chun-Yuen,Yip SenPo,Ho Johnny C.
Maximizing metal-substrate interactions by self-reconstruction of coadjutant metastable phases can be a delicate strategy to obtain robust and efficient high-density single-atom catalysts. Here, we prepare high-density iridium atoms embedded ultrathin CoCeOOH nanosheets (CoCe-O-Ir SA ) by the electrochemistry-initiated synchronous evolution between metastable iridium intermediates and symmetry-breaking CoCe(OH) 2 substrates. The CoCe-O-Ir SA delivers an overpotential of 187 mV at 100 mA cm −2 and a steady lifespan of 1000 h at 500 mA cm −2 for oxygen evolution reaction. Furthermore, the CoCe-O-Ir SA is applied as a robust anode in an anion-exchange-membrane water electrolysis cell for seawater splitting at 500 mA cm −2 for 150 h. Operando experimental and theoretical calculation results demonstrate that the reconstructed thermodynamically stable iridium single atoms act as highly active sites by regulating charge redistribution with strongly p - d - f orbital couplings, enabling electron transfer facilitated, the adsorption energies of intermediates optimized, and the surface reactivity of Co/Ce sites activated, leading to high oxygen evolution performance. These results open up an approach for engineering metastable phases to realize stable single-atom systems under ambient conditions toward efficient energy-conversion applications.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Xin Deng,Jinwei Chen,Qiuyan Chen,Yunzhe Zhou,Xinchi Liu,Jie Zhang,Gang Wang,Ruilin Wang
The modification of Ir or oxygen vacancies (V o ) is a strategy to enhance the oxygen evolution reaction (OER) performance of heterogeneous nanocatalysts. However, it is crucial to further clarify the synergistic effect of Ir and V o on the enhancement mechanism of OER performance after surface reconstruction. In this work, FeCo Layered double hydroxides (LDHs) co-modified by Ir and V o were successfully prepared by the thermodynamically favorable galvanic replacement reaction. Electrochemical impedance spectroscopy confirmed that the synergistic effect of Ir and V o enhanced the charge transfer of FeCo LDHs. XPS spectra reveal robust interactions between Ir and FeCo LDHs. Density-functional theory further reveals that the low-oxygen-coordinated Ir (III) acts as an active site to optimize the OER rate-determining step energy barrier. As a result, Ir and V o co-modified FeCo LDH requires only a 203 mV overpotential to achieve a current density of 10 mA cm −2 and, more importantly, operates stably at an industrial current density of 250 mA cm −2 for 312 h without degradation. This work provides new insights and avenues for understanding the enhanced performance mechanism of catalysts after surface reconstruction and for industrial scale-up production.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ANALYST
·
2012
·Vol. 137
·期 22
·5398-5402
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IF 4.23
Qun-bo Mei,Yuan-hui Guo,Bi-hai Tong,Jie-Na Weng,Bin Zhang,Wei Huang
A new phosphorescent chemosensor for Hg2+ and acetonitrile (MeCN) based on iridium(III) complex Ir(dpp)2(dtc) (Ir1, dppH = 4,6-diphenylpyrimidine, dtcH = diethyl dithiocarbamic acid) was realized. Upon addition of a tetrahydrofuran (THF) solution of Hg2+, the dichloromethane (DCM) solution of Ir1 gave a visual color change and significant fluorescent quenching. When MeCN was added, a new fluorescent emission emerged, which constituted a selective MeCN phosphorescent chemosensor. Complex Ir1 has been developed as an AND logic gate with Hg2+ and MeCN as inputs.
研究领域:
分析化学
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配位化学
✓ 已验证
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2018
·Vol. 5
·期 5
·1121-1125
·
IF 5.106
Luhong Fu,Xiang Zeng,Chaozhang Huang,Ping Cai,Gongzhen Cheng,Wei Luo
The exploration of highly active catalysts with superior stability for overall water splitting has received considerable attention. Although intensive efforts have been made to design numerous electrocatalysts for water splitting in alkaline media, only a few electrocatalysts have been developed for proton exchange membrane (PEM)-based electrolyzers in acidic media. Herein, we report a colloidal synthesis of well dispersed ultrasmall Ir NPs with narrow size distribution, of superior catalytic activity and stability toward HER and OER in acidic media. When further used as both an anode and a cathode for acidic overall water splitting, the as-synthesized monodisperse Ir NPs yield a current density of 10 mA cm−2 at 1.58 V with long-term stability.
研究领域:
材料科学
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电化学
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能源转换
✓ 已验证
DOI
高影响因子
INORGANICA CHIMICA ACTA
·
2024
·
IF 2.7
Zhen-Qiang Qin,Wen-Hao Li,Jia-Xin Zhang,Yi-Chuan Huang,Hong-Yan Li
Four cationic Ir(III) complexes Ir1–Ir4 , [(4-fpiq) 2 Ir(L 1 )]PF 6 ( Ir1 , 4-fpiq = 1-(4-fluorophenyl)isoquinoline, L 1 = 4,4′-dibromo-2,2′-bipyridine), [(4-fpiq) 2 Ir(L 2 )]PF 6 ( Ir2 , L 2 = 5,5′-dibromo-2,2′-bipyridine), [(4-chopiq) 2 Ir(L 1 )]PF 6 ( Ir3 , 4-chopiq = 1-(4-formylphenyl)isoquinoline), [(4-chopiq) 2 Ir(L 2 )]PF 6 ( Ir4 ) were synthesized using 2,2′-bipyridine derivatives as neutral ligands. These complexes show decent orange and red phosphorescence (λ em = 576–618 nm) with quantum efficiencies of 0.13–0.37. The influence of substituents in the ligands on the photophysical and electrochemical properties of the Ir(III) complexes was investigated by UV–vis absorption and emission spectra and cyclic voltammograms and simulated by density functional theory (DFT) calculations. Upon addition of OH − ions to the solutions of Ir1–Ir4 , all the complexes exhibited a turn-on response to OH − with a low detection limit on the order of 10 −6 M, and high selectivity to OH − was demonstrated.
研究领域:
分析化学
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配位化学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Huimin Zhang,Ping Song,Xuanhao Mei,Dezheng Zhang,Cong Liu,Mingtao Chu,Teng Zhang,Ce Han,Weilin Xu
Developing an efficient and stable bifunctional electrocatalyst for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in acidic media is of great significance, yet remains challenging. Herein, a bifunctional electrocatalyst supported by carbon cloth, denoted as IrNiOx/WO3, was designed and synthesized through heterostructured coupling of active amorphous IrNiOx with stable crystalline WO3. Benefiting from the pronounced electron interaction stemming from the as-generated numerous heterointerfaces, as-fabricated IrNiOx/WO3 demonstrates a low cell voltage of 1.539 V to achieve 10 mA cm–2 for water splitting with a low Ir loading of 0.8 wt % while maintaining stability over 100 h of continuous electrolysis in 0.5 M H2SO4. Furthermore, through comprehensive structural characterization and theoretical analysis, it was revealed that the Ir sites in the Ir–O–Ni configuration within amorphous IrNiOx serve as the primary active sites for both HER and OER processes. Moreover, the corresponding energy barriers were found to be significantly lowered due to the strong electronic interaction between amorphous IrNiOx and crystalline WO3. This study provides a strategy for designing amorphous–crystalline heterostructured electrocatalysts with ideal interfacial properties for efficient overall water splitting.
研究领域:
材料科学
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电化学
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yinghao Guo,Aiqing Cao,Lin Zhang,Marshet Getaye Sendeku,Yaping Li,Yun Kuang,Fengmei Wang,Xiaoming Sun
The chlorine evolution reaction is an anodic reaction in the chlor-alkali process, which utilizes dimensionally stable anodes (DSA) with large amounts of noble metals like iridium. Cheaper chlorine evolution anodes with high selectivity and stability are highly appealing but challenging. Here, a polymetallic oxide consisting of Sn, Ru, Nb, and Ti elements is synthesized on Ti felt for catalyzing chlorine evolution reaction. In particular, the Ru 0.3 Sn 0.6 Nb 0.1 O 2 film on Ti felt (i.e., Ru 0.3 Sn 0.6 Nb 0.1 O 2 /Ti) demonstrates a low overpotential of 42 mV at 10 mA cm −2 in 5 M NaCl (pH= 2) along with high Cl 2 selectivity (96.0 %) and mass activity (54.2 A g Ru −1 ) at 1.41 V versus reversible hydrogen electrode, which is 16 times higher than that of DSA electrode (3.2 A g Ru+Ir −1 ). Significantly, this anode can stably work for > 500 h at a current density of 100 mA cm −2 without attenuation. The flow cell fabricated with the Ru 0.3 Sn 0.6 Nb 0.1 O 2 /Ti anode and Pt/C cathode possesses excellent stability with a Cl 2 selectivity of 93 %, surpassing the flow cell fabricated with the DSA anode (81 %). The Ru 0.3 Sn 0.6 Nb 0.1 O 2 /Ti electrode exhibits low noble metal costs (7 % of DSA), and lower energy cost (82.5 % of DSA), but similar durability, showing great potential for industrial application.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shasha Li,Xunzhao Qiu,Xiaowei An,Enze Li,Xueyan Li,Guiru Wang,Peng Li,Caixia Shi,Yiming Liu,Guoqing Guan
Metal-organic frameworks (MOFs) derived spinel tricobalt tetroxide (Co 3 O 4 ) electrocatalysts incorporated with trifle Iridium (Ir) sites are in-situ grown on nickel foam (NF) substrate (Ir-Co 3 O 4 /NF) as effective anode for OER especially in near-pH-neutral seawater with high ability to suppress chlorine evolution reaction. Density functional theory (DFT) calculations indicate that the trifle Ir sites can be safeguarded in spinel Co 3 O 4 via structural-confinement and charge-redistribution so that the Ir and Co sites with their bridged electrophilic O ligands can serve as the active sites for boosting OER performance. As expected, a relatively low OER overpotential of 370 mV @ 10 mA cm −2 and it is achieved with at least 7 days durability under the current density of 100 mA cm −2 in near-pH-neutral simulated seawater with high selectivity toward OER. In same condition, a fabricated electrolyzer using it presents excellent electrocatalytic performance with a cell voltage of 2.11 V @ 100 mA cm −2 , strongly suggesting that the present electrolyzer has great promising for practical seawater electrolysis.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2022
·Vol. 20
·期 1
·1-17
·
IF 9.429
Wu Boda,Yang Jintao,Zu Yan,Chi Junjie,Shi Keqing
A film with elaborate microstructures that offers biomimetic properties and multi functionalities is highly desired in wound healing. Here, we develop an aligned hydrogel fiber film integrated with multi-active constituents to promote wound healing. Such fiber films are designed and constructed by photo-crosslinking the methacrylate gelatin (GelMA) doped with silver nanoparticles (Ag NPs) and iridium nanoparticles coated with polyvinylpyrrolidone (PVP-Ir NPs) in the precursor solution using electrospinning. The nature of GelMA hydrogel and the aligned arrangement of nanofibers endow the film with high-water content, self-degradability, improved bionic characteristics, oriented cell growth, and improved cell proliferation and migration. Moreover, the encapsulated nanozymes and Ag NPs offer the fiber film with superior reactive oxygen species (ROS) scavenging and antibacterial capability. The infected wound model shows that the multi-active hydrogel fiber film can reduce inflammation by killing bacteria and decomposing ROS, which accelerates the growth of new blood vessels and granulation tissue. Benefitting from these features, the versatile aligned GelMA fiber film demonstrates the clinically translational potential for wound healing.
研究领域:
材料科学
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生物医学工程
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纳米技术
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伤口愈合
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Wu Han,Chang Jiangwei,Yu Jingkun,Wang Siyang,Hu Zhiang,Waterhouse Geoffrey I. N.,Yong Xue,Tang Zhiyong,Chang Junbiao,Lu Siyu
The development of efficient and stable electrocatalysts for water oxidation in acidic media is vital for the commercialization of the proton exchange membrane electrolyzers. In this work, we successfully construct Ru–O–Ir atomic interfaces for acidic oxygen evolution reaction (OER). The catalysts achieve overpotentials as low as 167, 300, and 390 mV at 10, 500, and 1500 mA cm −2 in 0.5 M H 2 SO 4 , respectively, with the electrocatalyst showing robust stability for >1000 h of operation at 10 mA cm −2 and negligible degradation after 200,000 cyclic voltammetry cycles. Operando spectroelectrochemical measurements together with theoretical investigations reveal that the OER pathway over the Ru–O–Ir active site is near-optimal, where the bridging oxygen site of Ir–O BRI serves as the proton acceptor to accelerate proton transfer on an adjacent Ru centre, breaking the typical adsorption-dissociation linear scaling relationship on a single Ru site and thus enhancing OER activity. Here, we show that rational design of multiple active sites can break the activity/stability trade-off commonly encountered for OER catalysts, offering good approaches towards high-performance acidic OER catalysts.
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
Nano Energy
·
2024
·
IF 16.8
Wenxiang Zhu,Qintao Sun,Mengjie Ma,Fan Liao,Qi Shao,Hui Huang,Kun Feng,Dongdong Gao,Jinxin Chen,Hao Yang,Peiping Yu,Jun Zhong,Tao Cheng,Mingwang Shao,Yang Liu,Zhenhui Kang
Iridium (Ir) - based electrocatalysts, as the benchmark electrocatalysts for oxygen evolution reaction (OER), still suffer from sluggish kinetics and substantial overpotential. Here we show the fabrication of heterophase IrO 2 catalysts with homogeneous distribution of rutile phase on 1 T phase (referred to as m-IrO 2 ) by a simple air-annealing method. In acidic condition, the m-IrO 2 catalyst exhibits high activity with a low overpotential of 170 mV at 10 mA cm −2 and good stability with no sign of deactivation over a prolonged 508-h continuous operation, making it one of the best-performing acid-stable OER catalysts. In this system, H 2 O first forms OH* and O* on the rutile phase, and then the interfacial oxygen migrates from the rutile phase to the 1 T phase. Subsequently, O* drives the OER reaction on the 1 T phase, resulting in the generation of OOH* and eventually the formation of O 2 . The interfacial oxygen migration within the heterophase structure of m-IrO 2 boosts the acidic water oxidation activity significantly. These findings provide a promising design strategy for creating high-activity catalysts suitable for acidic conditions through the manipulation of interfaces.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Lan Yang,Hui Chen,Lei Shi,Xiaotian Li,Xuefeng Chu,Wei Chen,Nan Li,Xiaoxin Zou
One of the key objectives in PEM electrolysis technology is to reduce iridium loading and to improve iridium mass activity at the side of oxygen evolution electrocatalysis. 6H-phase, Ir-based perovskite (6H-SrIrO3) is known to be a promising alternative to the IrO2 catalyst, and developing effective strategies to further enhance its catalytic performance is needed. Here we present that a significant enhancement in electrocatalytic activity for the oxygen evolution reaction of 6H-SrIrO3 can be achieved by cobalt incorporation. A suitable amount of cobalt dopants results in a decreased formation temperature of 6H-SrIrO3 from 700 to 500 °C and thereby a decreased thickness of platelike particles for the material. Besides the morphological effect, the cobalt incorporation also increases the coverage of surface hydroxyl groups, regulates the Ir–O bond covalency, and modulates the oxygen p-band center of the material. This synergistic optimization of the morphological, surface, and electronic structures makes the cobalt-doped 6H-SrIrO3 catalyst give a 3-fold increase in iridium mass activity for oxygen evolution reaction in comparison with the undoped 6H-SrIrO3 under acidic conditions.
研究领域:
电化学
·
催化材料
·
能源材料
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）