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Nature Communications · 2018 ·Vol. 9 ·期 1 ·1-9 · IF 12.353

Efficient oxygen evolution electrocatalysis in acid by a perovskite with face-sharing IrO6 octahedral dimers

Yang Lan,Yu Guangtao,Ai Xuan,Yan Wensheng,Duan Hengli,Chen Wei,Li Xiaotian,Wang Ting,Zhang Chenghui,Huang Xuri,Chen Jie-Sheng,Zou Xiaoxin

The widespread use of proton exchange membrane water electrolysis requires the development of more efficient electrocatalysts containing reduced amounts of expensive iridium for the oxygen evolution reaction (OER). Here we present the identification of 6H-phase SrIrO 3 perovskite (6H-SrIrO 3 ) as a highly active electrocatalyst with good structural and catalytic stability for OER in acid. 6H-SrIrO 3 contains 27.1 wt% less iridium than IrO 2 , but its iridium mass activity is about 7 times higher than IrO 2 , a benchmark electrocatalyst for the acidic OER. 6H-SrIrO 3 is the most active catalytic material for OER among the iridium-based oxides reported recently, based on its highest iridium mass activity. Theoretical calculations indicate that the existence of face-sharing octahedral dimers is mainly responsible for the superior activity of 6H-SrIrO 3 thanks to the weakened surface Ir-O binding that facilitates the potential-determining step involved in the OER (i.e., O* + H 2 O → HOO* + H + +  e ¯ ).

CAS / MDL: 16920-56-2
研究领域: 材料科学 · 电化学 · 催化
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CHEMISTRY-A EUROPEAN JOURNAL · 2022 ·Vol. 28 ·期 68 ·e202202004 · IF 5.02

Bismuth Gadolinium Oxychloride with a Remarkable Visible-Light-Responsive O2 Evolution Activity Promoted by Iodine Doping

Conghui Zhao,Liwei Sun,Yang Xu,Beibei Dong,Yuhong Luo,Jingde Li,Jianxin Chen,Zisheng Zhang

Graphical Iodine-doped Bi 2 GdO 4 Cl with a significantly promoted visible-light-responsive O 2 -evolving performance of 154.8 μmol ⋅ h −1 and an apparent quantum efficiency of ∼1.1 % at 420 nm is reported. The incorporation of I − ions causes the extended light absorption and promoted charge separation. Visible-light-responsive bismuth-based oxyhalide has recently attracted extensive attention, however, the promotion of its charge separation is still challenging. Herein, we introduce iodine into Bi 2 GdO 4 Cl to synthetize I-doped Bi 2 GdO 4 Cl (denoted as yI−Bi 2 GdO 4 Cl, 0≤y≤2). The incorporation of I − ions is found to enhance light absorption and to accelerate charge separation by combining various characterizations such as density functional theory calculation, photoelectrochemical test, electrochemical impedance spectroscopy, photoluminescence spectrum, and open-circuit voltage decay. The O 2 -evolving performances of 1I−Bi 2 GdO 4 Cl with optimized dopant concentration of I − ion and IrO 2 loaded 1I−Bi 2 GdO 4 Cl are tremendously enhanced by ca. 4 and 45 times compared to pristine Bi 2 GdO 4 Cl. Notably, The O 2 evolution rate reaches as high as 154.8 μmol ⋅ h −1 with an apparent quantum efficiency of ∼1.1 % at 420 nm. The synthetic iodine-doped photocatalyst remains stable after long-term photoreaction, demonstrating its potential in the field of photocatalysis.

研究领域: 材料科学 · 光催化
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CHINESE JOURNAL OF CATALYSIS · 2018 · IF 3.525

Three-dimensional lily-like CoNi2S4 as an advanced bifunctional electrocatalyst for hydrogen and oxygen evolution reaction

Jingwei Li,Qiuna Zhuang,Peiman Xu,Dawei Zhang,Licheng Wei,Dingsheng Yuan

Designing low-cost, highly efficient, and stable bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of vital significance for water splitting. Herein, three-dimensional lily-like CoNi 2 S 4 supported on nickel foam (CoNi 2 S 4 /Ni) has been fabricated by sulfuration of the Co–Ni precursor. As expected, CoNi 2 S 4 /Ni possesses such outstanding electrocatalytic properties that it requires an overpotential of only 54 mV at 10 mA cm −2 and 328 mV at 100 mA cm −2 for HER and OER, respectively. Furthermore, by utilizing the CoNi 2 S 4 /Ni electrodes as bifunctional electrocatalysts for overall water splitting, a current density of 10 mA cm −2 can be obtained at a voltage of only 1.56 V.

研究领域: 材料科学 · 能源化学
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Nano Energy · 2019 · IF 15.548

Monolithic electrode integrated of ultrathin NiFeP on 3D strutted graphene for bifunctionally efficient overall water splitting

Rui-Qing Li,Bao-Lu Wang,Tian Gao,Ran Zhang,Chenyang Xu,Xiangfen Jiang,Jinjue Zeng,Yoshio Bando,Pengfei Hu,Yongle Li,Xue-Bin Wang

High-performance earth-abundant electrocatalysts for oxygen and hydrogen evolutions are highly desired for renewable energy but remain challenging. Herein, we have developed ultrathin NiFeP nanosheets , and merged the NiFeP with a 3D support of sponge-like strutted graphenes (SG). The synthesized NiFeP/SG, a porous monolith, shows efficient electrocatalytic activities for oxygen and hydrogen evolutions in alkaline electrolyte with low overpotentials of 218 and 115 mV, respectively. Using NiFeP/SG as direct catalytic electrodes, the overall water splitting requires a low cell voltage of 1.54 V to achieve a current of 10 mA cm −2 . The high performances result from the shifted-up d states caused by iron incorporation, the ultrathin NiFeP, and the 3D network structure of SG. Additionally, NiFeP/SG demonstrates excellent gravimetric catalytic activities , meaningful to aerospace and portables. The material opens the way to a universal robust lightweight catalytic electrode for a variety of applications in electrochemical energy storage and conversion .

研究领域: 材料科学 · 能源化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2015 ·Vol. 163 ·期 3 ·E33 · IF 3.266

Electrochemical Metallurgy in CaCl2-CaO Melts on the Basis of TiO2·RuO2 Inert Anode

Liwen Hu,Yang Song,Jianbang Ge,Shuqiang Jiao,Jin Cheng

Molten CaCl2 has been considered as significant electrolyte for novel electrochemical metallurgy processes due to high solubility of oxygen anions. Some novel processes based on molten-salt electrolysis of oxides in molten chlorides have been proposed, typically including FFC process and OS process. An inert anode capable of sustained oxygen evolution is crucial for a green and efficient electrochemical de-oxidation process. Herein we report the results of a promising inert anode candidate, who shows an excellent performance. Several techniques including anodic polarization, cyclic voltammetry, Tafel polarization and electrochemical impedance have been performed to evaluate the anode behavior of the TiO2·RuO2 anode, revealing that the anode is quite stable during anodic polarization and has a more positive corrosion electrode potential. An in situ analysis of anode gases using the mass spectra proved the capability of the sustained evolution of oxygen at the TiO2·RuO2 anode during electrolysis, meaning that this oxides anode could be a potential candidate as inert anode in calcium chloride–calcium oxide melts for green metallurgical processes, as it showed a nearly negligible solubility of ruthenium dioxide when immersed in the melt and a low rate of corrosion even after long time electrolysis.

CAS / MDL: 12036-10-1
研究领域: 冶金学 · 电化学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Crown ether as a bifunctional booster in electrochemical water splitting

Yanan Chen,Luofu Min,Wen Zhang,Li Xu,Yuxin Wang

Electrochemical water splitting using renewable energy is considered a key technology to mitigate global warming and to realize the hydrogen economy . Extensive efforts have been devoted to finding high-performance electrode catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) involved in electrochemical water splitting, whereas the research on added components in the electrolyte to boost HER and/or OER is very limited. In this work, we report the use of 18-crown ether-6 (18C6) in the electrolyte as a bifunctional booster in water splitting. The addition of 18C6 in alkaline electrolyte drastically boosts HER current density from −50 to −300 mA cm −2 at −0.3 V vs. RHE and OER current density from 25 to 250 mA cm −2 at 1.7 V vs. RHE on the Ni foam electrode. Combing DFT calculations and experimental characterizations, the functions of 18C6 in boosting HER and OER on nickel electrodes under the alkaline condition are revealed. This research demonstrates the potential of macrocycle molecules as electrolyte additives and opens up new opportunities for boosting the performance of water splitting.

研究领域: 材料科学 · 电化学 · 可再生能源
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

NiCo layered double hydroxides derived Ni0.67Co0.33(PO3)2 as stable and efficient electrocatalysts for overall water splitting

Shuo Geng,Yarong Huang,Akhmat Fauzi,Yongsheng Yu,Yequn Liu,Weiwei Yang

The synthesis of highly efficient non-noble bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in the same electrolyte is important for the industrial application of electrocatalytic water splitting. Herein, non-noble bifunctional electrocatalyst Ni 0.67 Co 0.33 (PO 3 ) 2 nets with optimized morphology were successfully synthesized. Owing to the micropores with the accelerated electrolyte and gases transfer and nanopores architecture with more exposed active edge sites, the self-supported Ni 0.67 Co 0.33 (PO 3 ) 2 -12 h electrode exhibits a superior water splitting performance. Impressively, the Ni 0.67 Co 0.33 (PO 3 ) 2 -12 h electrode only needs a cell voltage of 1.46 V to achieve 10 mA/cm 2 and shows over 22 h stability at 10, 50 and 100 mA/cm 2 , respectively. This present work suggests a unique and earth abundant material synthesis method for water electrolysis, which has broad prospects for practical water splitting application.

研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

CeO2 as an “electron pump” to boost the performance of Co4N in electrocatalytic hydrogen evolution, oxygen evolution and biomass oxidation valorization

Peiyun Zhou,Guangtong Hai,Gongchi Zhao,Rushuo Li,Xiubing Huang,Yunfeng Lu,Ge Wang

Developing multifunctional electrocatalysts with excellent hydrogen evolution reaction (HER), oxygen evolution reaction (OER) and 5-hydroxymethylfurfural oxidation reaction (HMFOR) activities will contribute to "carbon neutrality". Here, CeO 2 is introduced into the Co 4 N system as an "electron pump" to attract electrons to transfer from Co 4 N to CeO 2 . The interface electronic structure optimization enables Co 4 N@CeO 2 to exhibit excellent HER, OER, and HMFOR performance. Specifically, to deliver 10 mA cm −2 current density, (1) it only requires low overpotentials of 49 and 263 mV for HER and OER in 1.0 M KOH, respectively; (2) it merely needs an ultra-low potential of 1.22 V RHE for HMFOR in 1.0 M KOH + 300 mM HMF, which is 273 mV lower than the required potential in 1.0 M KOH. Theoretical calculation results show that the introduction of CeO 2 effectively reduces the barriers for potential-determining steps of HER and OER, and optimizes OH - adsorption to promote the HMFOR process.

研究领域: 材料科学 · 能源化学
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ENERGY & FUELS · 2022 · IF 4.654

Effect of the Valence State in Co-Based Cocatalyst on the Photocatalytic Oxygen Evolution Reactivity of WO3

Yongshuo Yang,Qiqi Zhang,Xinmin Yang,Huilin Hu,Lequan Liu,Jinhua Ye,Defa Wang

WO3 is one of the most promising photocatalysts with a suitable energy band structure for water oxidation; however, the quick recombination of photoinduced charge carriers seriously limits the photocatalytic efficiency. Loading of suitable cocatalysts is considered as an effective method to significantly improve the photocatalytic activity. Herein, we used a facile one-step hydrothermal method and a “hydrothermal + photodeposition” method to synthesize xCo3O4/WO3 (x = 0.2, 0.4, 0.8) and yCoOOH/WO3 (y = 2, 3, 4), respectively. We found that, in comparison with the pristine WO3, both xCo3O4/WO3 and yCoOOH/WO3 exhibited remarkably increased photocatalytic O2 evolution activities owing to the loading of two Co-based cocatalysts Co3O4 and CoOOH, respectively. Moreover, the optimal O2 evolution rate achieved over 0.4Co3O4/WO3 (194 μmol·h–1) was ∼2.1 times that over 3CoOOH/WO3 (94 μmol·h–1). The superior photocatalytic O2 evolution activity of Co3O4/WO3 over CoOOH/WO3 could be attributed to the mixed valences of Co2+ and Co3+ in Co3O4, which was more favorable than CoOOH with the sole valence of Co3+ for promoting the separation and transfer of photoinduced electrons and holes. This work suggests a promising way to the development of noble-metal-free cocatalyst by using transition-metal oxide with mixed valence states for efficient photocatalytic water oxidation.

CAS / MDL: 10213-10-2
研究领域: 材料科学 · 化学 · 催化 · 环境科学
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ADVANCED MATERIALS · 2024 ·Vol. 37 ·期 4 ·2411510 · IF 27.4

Lab-on-Fiber Operando Deciphering of a MOF Electrocatalyst

Tiansheng Huang,Li-Peng Sun,Xiangping Li,Bai-Ou Guan

Despite the great success in deploying metal-organic frameworks (MOFs) as efficient electrocatalysts, the low adoption of operando methods hinders the understanding of underlying mechanism. By leveraging the subtle refractive index evolution, including both the real and the imaginary parts, an entirely new concept of a lab-on-fiber operando method and its feasibility for “pristine-immersion-operando-post analysis” of electrocatalyts are demonstrated. Concurrent collection of absorption spectra and surface plasmon resonance is achieved by engineering fiber-optic waveguides to simultaneously induce guided light attenuation and plasmonic coupling. In situ-formed Co hydroxide and oxide reactive intermediates in zeolitic imidazolate framework-67 (ZIF-67) electrocatalyst are optically identified, which shows its underlying self-reconstruction conversions at different stages during electrocatalytic oxygen evolution reactions, and address the gap in knowledge concerning whether ZIF-67 is a precatalyst for real catalyst production. This illuminating operando method offers intriguing opportunities to collect all the observables in a single fiber, provides an exciting potential of a new class of device with long-sought integration and miniaturization capability, and is expected to enable the electrocatalysis community to conquer challenges with conducting multimodal operando experiments outside the laboratory.

CAS / MDL: 57-09-0
研究领域: 材料科学 · 电化学 · 光学工程
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

Efficiently suppressing oxygen evolution in high voltage graphite/NCM pouch cell with tributyl borate as electrolyte additive

Jianhui Li,Xuerui Yang,Xiongcong Guan,Rude Guo,Yanxia Che,Jianlian Lan,Lidan Xing,Mengqing Xu,Weizhen Fan,Weishan Li

Energy density of lithium ion batteries based on transition metal oxide cathodes can be enhanced by increasing the end-off charge voltage to a great extent, because the cathodes can deliver a larger specific discharge capacity under an elevated charge voltage. However, this operation is always accompanied by the oxygen evolution from the cathode oxides, which might cause the crystal destruction of the cathode oxides and the severe electrolyte decomposition on the cathodes, leading to the fast failure of the batteries . In this work, we report a new finding that the oxygen evolution in graphite/LiNi 0.6 Mn 0.2 Co 0.2 O 2 pouch cell can be efficiently suppressed and thus the cyclic stability of the cell is significantly improved by using tributyl borate (TBB) as electrolyte additive , even under 4.5 V. Electrochemical tests indicate that, with adding 1 wt% TBB to the electrolyte, the capacity retention of the cell is enhanced from in 35.1% to 94.9% after 120 cycles. The physical characterizations combining theoretical calculations demonstrate that the B-containing species in the cathode electrolyte interphase, originated from the oxidation of TBB, present a strong combination with oxygen and suppress efficiently the oxygen evolution.

CAS / MDL: 17374-26-4
研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Single-Step and Room-Temperature Synthesis of Laser-Induced Pt/VC Nanocomposites as Effective Bifunctional Electrocatalysts for Hydrogen Evolution and Oxygen Evolution Reactions

Nan Wang,Xiangjie Bo,Ming Zhou

The development of cost-effective Pt-based electrocatalysts is of great scientific and industrial significance for improving the electrocatalytic activity of hydrogen evolution (HER) and oxygen evolution (OER) reactions for overall water splitting. In this work, unlike traditional furnace pyrolysis, we report the rapid and single-step room-temperature synthesis of Pt/VC nanocomposites with a three-dimensional (3D) network porous structure by laser irradiation technology. The resultant Pt-based composite (Pt/VC-2.84) could be applied to HER under different pH conditions. In particular, the content of Pt in Pt/VC-2.84 is only 2.84 wt %, which is far lower than that in the advanced HER electrocatalyst with the Pt content of 20 wt % (commercial 20 wt % Pt/C). In addition, Pt/VC-2.84 exhibits a boosted higher OER activity and stability than RuO2 in an alkaline medium. Most importantly, electrocatalytic results reflect that Pt/VC-2.84 reveals superior activity and stability toward overall water splitting.

研究领域: 材料科学 · 电化学
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