Nano Research
·
2023
·
IF 9.9
Ni Jing,Shi Zhaoping,Wang Yibo,Yang Jiahao,Wu Hongxiang,Wang Pengbo,Li Kai,Xiao Meiling,Liu Changpeng,Xing Wei
The scale-up deployment of ruthenium (Ru)-based oxygen evolution reaction (OER) electrocatalysts in proton exchange membrane water electrolysis (PEMWE) is greatly restricted by the poor stability. As the lattice-oxygen-mediated mechanism (LOM) has been identified as the major contributor to the fast performance degradation, impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative, yet remains challenging due to the lack of efficient approaches. Herein, we strategically regulate the bonding nature of Ru-O towards suppressed LOM via Ru-based high-entropy oxide (HEO) construction. The lattice disorder in HEOs is believed to increase migration energy barrier of lattice oxygen. As a result, the screened Ti 23 Nb 9 Hf 13 W 12 Ru 43 O x exhibits 11.7 times slower lattice oxygen diffusion rate, 84% reduction in LOM ratio, and 29 times lifespan extension compared with the state-of-the-art RuO 2 catalyst. Our work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.
研究领域:
材料科学
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电化学
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催化
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能源材料
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2021
·Vol. 45
·期 10
·15544-15556
·
IF 5.164
Xuerui Yi,Fengxiang Yin,Xiaobo He,Guoru Li
Summary Water splitting driven by renewable energy represents a sustainable way to store clean energy. However, its efficiency is limited by the kinetically sluggish oxygen evolution reaction (OER), calling for highly active catalysts to accelerate the reaction rate. Herein, NiO is reduced by cellulose through a hydrothermal method to obtain the highly active OER catalysts. The obtained cellulose-partially-reduced-NiO (CL-prNiO) shows a hybrid structure, composed of 3.6 wt.% face-centered cubic (fcc) Ni and 96.4 wt.% rock salt structured NiO with highly disordered interface. The CL-prNiO delivers a current density of 10 mA cm −2 with an overpotential of 288 mV, which is comparable to the commercial RuO 2 and outperforms many of the recently reported Ni-NiO based OER catalysts. As benefited from the hybrid and disordered structure, CL-prNiO shows great ability of converting Ni 2+ to Ni 3+ at a potential prior to the OER onset. The in situ generated Ni 3+ species can activate the lattice oxygen in the unreduced NiO of CL-prNiO, significantly boosting the OER activity.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2022
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IF 6.959
Yuling Zhang,Juan Zhang,Qianying Yi,Fengliang Wang,Hongquan Fu,Hejun Gao,Yunwen Liao
Photocatalytic nitrogen fixation is considered as a multielectron reaction and a complex kinetic process, building high-performance nitrogen fixation photocatalysts to solve the activation of N2 and inhibit the recombination of photogenerated holes and electrons under the visible light condition. Herein, porous β-Bi2O3/BiOCOOH heterojunction photocatalysts with oxygen vacancies were prepared via BiOCOOH as a sacrificial precursor by the calcination method. The as-obtained β-Bi2O3/BiOCOOH catalyst with oxygen vacancies exhibited a high catalytic activity of about 65.56 μmol·g–1·h–1 for N2 fixation via deionized water as a solvent and methanol as a sacrificial agent. Both experimental and theoretical research indicated that the activity of β-Bi2O3/BiOCOOH heterojunction catalysts originated from the oxygen vacancies and lattice oxygen species. Compared to the single-component BiOCOOH structure, the porous β-Bi2O3/BiOCOOH heterojunction catalysts have achieved the absorption visible light range and have promoted the separation efficiency of charge carrier pairs by accommodating photogenerated electrons. Our findings afford a chance to improve a promising catalyst for photocatalytic nitrogen fixation.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Juanjuan Feng,Yu Tian,Kunlin Li,Fei Wang,Kai Li,Ping Ning
Toxic H 2 S limits the high-value utilization of high-concentration CO in yellow phosphorus tail gas. High-performance adsorbents play a significant role in the purification of yellow phosphorus tail gas and the recovery of CO. In this study, manganese-based adsorbents doped with other metals (Cu, Co, Ni, Ce, and Fe) were synthesized and tested for H 2 S removal. The results demonstrate that doping α-MnO 2 with metals significantly enhances its desulfurization performance. Notably, the 20 % Ni/Mn adsorbent achieves the best performance, exhibiting an adsorption duration of approximately 50 h under test conditions and H 2 S capacity up to 854.35 mg/g. Mechanism studies show that the performance improvement is mainly attributed to the doping of Ni, which disrupts the growth of the α-MnO 2 rod-like structure, promoting the formation of fine particles and exposing more crystal interfaces. This is conducive to the migration and release of active lattice oxygen species on the adsorbent, thereby enhancing the adsorption-oxidation performance of the adsorbent for H 2 S. Moreover, Ni significantly promotes the formation of high-valent Mn, enhancing the adsorbent’s oxidation capability and facilitating the decomposition of H 2 S. This study proposes an innovative synthetic strategy for constructing adsorbents with high H 2 S adsorption performance under anaerobic and dry conditions.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2024
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IF 6.5
Fuping Song,Juping Zhang,Dongfang Li,Tao Zhu,Xing Zhu,Hua Wang
Oxidative dehydrogenation (ODH) of ethylbenzene is a promising process for styrene production. However, its application is limited by product overoxidation and purification requirements due to the co-feeding of mild oxidants. Herein, we report a facile manganese-based catalyst (K/Mn 3 O 4 -Al 2 O 3 ) and achieve competitive styrene selectivity of 88 % and ethylbenzene conversion of 95 % at 450 ℃ (84 % yield vs. ∼ 60 % yield in commercial dehydrogenation process at 600 ℃) under a cyclic redox ODH scheme. The introduction of Al 2 O 3 into MnO x restructures composite oxides and depresses bulk lattice-oxygen migration for the partial oxidation of ethylbenzene. The surface modification using potassium creates reactive sites and regulates surface properties, achieving ethylbenzene activation and high conversions. Highly active lattice oxygen in catalysts after bulk and surface modifications selectively converts ethylbenzene to styrene and water. This study provides an understanding of roles of manganese-based catalysts in styrene generation and offers a strategy to modulate lattice oxygen on catalysts.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2019
·Vol. 33
·期 3
·e4745
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IF 3.259
Yibing Xie,Langlang Wang,Ping Ning,Xueqian Wang,Qi Wang,Yingjie Zhang,Mengyu Wang
A series of Ce modified catalysts were prepared using equivalent-volumetric ultrasonic impregnation method for AsH 3 removal. The performance of catalytic oxidation of AsH 3 under dynamic conditions was studied under different synthesis and reaction conditions. Through screening tests, the optimum catalyst was impregnated by 10 wt.% Ce (CH 3 COO) 3 precursor and subsequently calcinated at 550 °C. When the reaction temperature reached 170 °C, the Ce-HZSM-5 catalyst could maintain an oxidation efficiency of over 90% in 82 hrs. Furthermore, the chemical structure and properties of the catalyst and its catalytic oxidation mechanism with AsH 3 were analyzed using SEM-EDS, BET, XRD, XPS, H 2 -TPR and FT-IR. The results showed that Ce mainly existed on the catalyst surface in the forms of Ce 4+ and Ce 3+ . In the reaction process, the chemisorbed oxygen played a key role in the transformation between the two valence states. AsH 3 was firstly oxidized to elemental As with the participation of lattice oxygen. Then, the elemental As was partially blown into the rear part of the adsorption column along with the air flow and subsequently, de-sublimed on the column wall. Herein, the elemental As remained on the surface of Ce-HZSM-5 catalyst, which would further oxidize to As 2 O 3 . For the recovery of As, Ce-HZSM-5 proved to be a promising catalyst in AsH 3 removal. Highlights The CeO x modified HZSM-5 catalyst was used to catalytic oxidation of AsH 3 . The Ce-HZSM-5 catalyst could maintain over 90% oxidation efficiency in 82 hrs. AsH 3 was catalytic oxidized to elemental As and H 2 O on the catalyst surface and the As can be collected. The As adsorbed on the catalyst surface can be oxidized to As 2 O 3 but cannot be further oxidized to As 2 O 5 .
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2023
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IF 7.3
Lei Wang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Jie Ding,Li Zhu,Jing Ma,Wenxin Ji,Liqiong Wang,Yuanyuan Li
Dual activation of molecular and lattice oxygen is an important step in the catalytic oxidation of volatile organic compounds. Herein, CeO 2 was derived from MOF as an electron donor support to develop a co-catalyst with Pt-Pd alloy nanoparticles (Pt-Pd/CeO 2 ). The Prepared Pt-Pd/CeO 2 exhibits excellent catalytic activity towards toluene oxidation, showing a turnover frequency (TOF 0.26 s −1 ) higher than those of Pt/CeO 2 (0.05 s −1 ) and Pd/CeO 2 (0.02 s −1 ). Several in situ experimental techniques and density functional theory calculations have revealed that the introduction of Pd valence electrons can intensify the electronic metal-support interactions (EMSIs) effects of Pt-Pd/CeO 2 catalysts, which can weaken the Ce-O bond, thereby promoting the production and circulation of lattice oxygen and oxygen vacancies, and modulating the d -band centre to enhance the adsorption and activation of reactants. This study presents a comprehensive investigation of toluene oxidation on alloy-supported catalysts, providing practical guidance for designing reliable catalysts suitable for industrial applications.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
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2024
·
IF 14.3
Yang Peng,Xu Zhao,Yiqun Shao,Xin Yue,Zhuofeng Hu,Shaoming Huang
Spinel-type nickel ferrite (Ni x Fe 3-x O 4 , x≤1) is a widely used electrocatalyst for the oxygen evolution reaction (OER). Due to the lower hybridization of metal- d and oxygen- p orbitals, the OER process on Ni x Fe 3-x O 4 follows the sluggish adsorbate evolution mechanism (AEM). Generally, activating the lattice oxygen to trigger the lattice-oxygen-mediated mechanism (LOM) can enhance the OER activity. Herein, to trigger the LOM pathway while maintaining high stability, iron foam (IF)-supported Ni 0.75 Fe 2.25 O 4 (NiFeO) with geometrical defects of [NiO 6 ] (nickel cation coordinated with six oxygen anions) units and higher ratio of Fe to Ni cations in octahedral sites ( d -NiFe HR O/IF) is prepared by ion-exchanging with polar aprotic solvent followed by annealing. As a result, as-synthesized d -NiFe HR O/IF exhibits excellent activity (at 295 mV overpotential to achieve 100 mA cm −2 ), fast kinetics (Tafel slope of only 34.6 mV dec −1 ), and high stability (maintaining a current density of 100 mA cm −2 over 130 h) for the OER. The theoretical calculations reveal that the construction of octahedral defect in Ni x Fe 3-x O 4 enhances the overlap of Fe- d and O- p orbitals, which can activate the lattice oxygen. Therefore, increasing the ratio of Fe to Ni will further improve the lattice oxygen redox activity, and thus trigger the fast LOM pathway, ultimately facilitating the OER process.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Jiangyu Tang,Xiao Wang,Yunfa Wang,Min Shi,Peng Huo,Jianxiang Wu,Qiaoxia Li,Qunjie Xu
The oxygen evolution reaction (OER) serves as a fundamental half–reaction in the electrolysis of water for hydrogen production, which is restricted by the sluggish OER reaction kinetics and unable to be practically applied. The traditional lattice oxygen oxidation mechanism (LOM) offers an advantageous route by circumventing the formation of M-OOH* in the adsorption evolution mechanism (AEM), thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order. Fortunately, the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen, which could be activated by rational band structure design for direct O-O coupling, where the M–O bond maintains its initial bond order. Here, non-bonding oxygen was introduced into NiFe 2 O 4 via annealing in an oxygen-deficient atmosphere. Then, in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons, thereby facilitating the transformation of the redox center from metal to oxygen. LOM based on non-bonding oxygen (LOM NB ) was successfully activated within NiFe 2 O 4 , exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm –2 and excellent durability of stable operation for over 150 h. Additionally, catalysts featuring varying band structures were synthesized for comparative analysis, and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2 p holes are critical prerequisites for triggering and sustaining the LOM NB pathway in transition metal spinel oxides. These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.
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
高影响因子
ACS Catalysis
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2022
·
IF 13.7
Chang Sun,Pengcheng Zhao,Yongqing Yang,Zhuo Li,Wenchao Sheng
The application of anion exchange membrane fuel cells is hampered by the development of highly efficient and earth-abundant anode hydrogen oxidation reaction (HOR) catalysts. Here, a series of nickel catalysts (denoted as Ni-X) with different lattice oxygen (LO) contents were synthesized by H2 reduction of nickel hydroxide at temperatures (X) ranging from 300 to 500 °C. The Ni-400 (LO/Ni = 0.41, NiO0.41) catalyst with an optimum LO content showed excellent HOR activity and stability, comparable to current Ni-based electrocatalysts. An X-ray photoemission spectroscopic study, combined with density functional theory calculations, suggested that introducing LO into Ni modified the metal d-band electronic structure and in turn the hydrogen binding energy, which played a major role in determining the HOR performance.
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
Journal of Cleaner Production
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2023
·
IF 11.1
Lujie Zuo,Shufan Yu,Rongjun Zhang,Hongwei Li,Yu Wu,Rufat Abiev,Zhao Sun,Zhiqiang Sun
Methanol is a competitive candidate for in-situ hydrogen supply; however, the techniques of methanol-to-hydrogen production are suffered from high reforming temperatures and catalyst deactivation . In this work, the chemical looping oxidative reforming of methanol is conducted using a Pd–Cu-based catalytic oxygen carrier (PdO–CuO–CuMn 2 O 4 ). Synergistic enhancement of lattice oxygen induction and Pd–Cu alloy activation is confirmed, thereby achieving efficient methanol reforming at a temperature as low as 200 °C. Under such low temperatures, the hydrogen production rate can reach an average of 11.2 times higher than that of CuO/ZnO/Al 2 O 3 . Moreover, the catalytic oxygen carrier remains relatively satisfying redox durability after 30th cycle. SEM and AFM measurements reveal the high degree of roughness at the PdO–CuO–CuMn 2 O 4 surface, in which the methanol activation can be effectively promoted. XRD and XPS measurements verify the formation of Pd–Cu alloy, as proved by the charge transfer from Pd to Cu. During the redox looping, Pd–Cu alloy is formed and re-separated to be PdO and CuO, thus remaining homogenous distribution of the active phase on an atomic scale. Meanwhile, the lattice oxygen also plays a crucial role in methanol activation, synergistically enhancing the low-temperature reforming of methanol. This study provides a new implication for designing functionalized catalytic oxygen carrier materials , which will substantially promote in-situ hydrogen supply for proton exchange membrane fuel cells.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 10
·1181
·
IF 4.501
Da Song,Yan Lin,Kun Zhao,Zhen Huang,Fang He,Ya Xiong
CO2resourceful utilization contributes to the goal of carbon neutrality. Chemical Looping Dry Reforming (CLDR) has attracted significant attention as a method for converting CO2to CO. NiFe2O4oxygen carrier (OC) is found to be a potential material for CLDR. However, the migration process of lattice oxygen, which are critical for the conversion of CO2to CO, was not extensively investigated. In this study, the reduction and oxidation degrees of the NiFe2O4were finely modulated in a thermogravimetric analyzer. The lattice oxygen migration mechanism of the NiFe2O4in redox cycles was characterized by means of X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and in-situ Raman. The novelty of this paper is clarifying the release-uptake paths of lattice oxygen during CO2resourceful utilization. The result indicates that the concentration gradient between the surface and the bulk drives the diffusion of lattice oxygen. The stabilization of surface lattice oxygen content is attributed to the rapid migration of O anion, which is closely associated with the movement process of Ni particles inward and outward through the spinel bulk. In addition, a highly reactive chemical reaction interface consisting of lattice oxygen and the corresponding metal atoms is always present on the surface of the oxygen carrier and is confirmed by an in-situ Raman and XPS during the whole process of CLDR. The results of this paper offer reference and basis for further development and design of CLDR using spinel OC.Keywords:chemical looping (CL);oxygen carrier (OC);CO2splitting;lattice oxygen;NiFe2O4
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）