Nature Communications
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2024
·Vol. 15
·期 1
·1-11
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IF 14.7
Du Yu,Xie Fakang,Lu Mengfei,Lv Rongxian,Liu Wangxi,Yan Yuandong,Yan Shicheng,Zou Zhigang
Compressive strain, downshifting the d -band center of transition metal oxides, is an effective way to accelerate the sluggish kinetics of oxygen evolution reaction (OER) for water electrolysis. Here, we find that anisotropic thermal expansion can produce compressive strains of the IrO 6 octahedron in Sr 2 IrO 4 catalyst, thus downshifting its d- band center. Different from the previous strategies to create constant strains in the crystals, the thermal-triggered compressive strains can be real-timely tuned by varying temperature. As a result of the thermal strain accelerating OER kinetics, the Sr 2 IrO 4 exhibits the nonlinear ln j o - T −1 ( j o , exchange current density; T , absolute temperature) Arrhenius relationship, resulting from the thermally induced low-barrier electron transfer in the presence of thermal compressive strains. Our results verify that the thermal field can be utilized to manipulate the electronic states of Sr 2 IrO 4 via thermal compressive strains downshifting the d -band center, significantly accelerating the OER kinetics, beyond the traditional thermal diffusion effects.
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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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yuhua Xie,Yumei Feng,Chen Li,Fang Luo,Qing Li,Shiao Zhu,Mingxing Gong,Zehui Yang
The industrial development of acidic water splitting significantly counts on the activity associated with stability of oxygen evolution reaction (OER) electrocatalyst. In this work, we have constructed cubic Rh@Ir core–shell for acidic water splitting. The formed Rh@Ir electrocatalyst shows a high HER performance with only 29 mV overpotential for 10 mA cm −2 , stemming from the upshifted and downshifted d band center of Ir and Rh, leading to a moderate hydrogen binding strength. The Ir atom donates its electrons to nearby Rh atoms triggering a high susceptibility in nucleophilic attack by H 2 O to generate *OOH; thereby, the overpotential required to achieve 10 mA cm −2 is 216 mV for Rh@Ir core–shell, better than commercial IrO 2 . Moreover, the stability is superior to commercial IrO 2 and pure Ir electrocatalyst due to the strong electronic interplay in Rh@Ir contributing to a better resistance towards electrochemical dissolution proved by operando Raman and electrochemical impedance spectroscopies. Only 1.55 V is needed for Rh@Ir to drive overall water splitting at 10 mA cm −2 .
研究领域:
电化学
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材料科学
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催化
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2024
·Vol. 59
·期 15
·6270-6284
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IF 3.5
Wu Hongmei,Liu Baoshan,Zhang Yao,Li Feng,Liu Jing,Zhao Liping,Zhang Peng,Gao Lian
Cobalt-based transition metal phosphides (TMPs) exhibit huge potential as efficient OER electrocatalysts for commercial applications. Zeolitic imidazolate framework-67 (ZIF-67) has been served as an appealing precursor for the synthesis of cobalt-based TMPs owing to its distinctive structural advantages. However, the poor conductivity and structural variability of ZIF-67 affect the materials’ OER electrocatalytic performance. To enhance the structural stability and OER performance of ZIF-67 derived TMPs, in this work, a polyhedral TMP nanocomposite with porous hollow structure, featuring Fe-CoP on the outer shell and CoP nanoparticles within the cavity, was synthesized using ZIF-67 as template. The ZIF-67 served as both Co precursor and structure template, and the [Fe(CN) 6 ] 3− served as precursor of Fe dopant and structure stabilizer. The resulting TMP composite electrode (Fe-CoP) effectively retains the framework of ZIF-67, exhibiting prominently improved OER activity (η 10 = 297 mV) and exceptional stability (over 260 h). The Fe–C≡N–Co bonds positively influence the preservation of the sample’s morphology after phosphorization. Additionally, a ligand-substitution strategy is proposed for the formation of the designed structure. This strategy, regulating the morphology of 3D structured MOFs, offers a new understanding on stabilizing the geometric structure of MOFs and their derivatives as structure templates. Graphical abstract
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
APPLIED SURFACE SCIENCE
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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
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
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2021
·Vol. 105
·期 4
·2690-2701
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IF 3.784
Lu Zou,Zhao Lu,Ziling Wang,Bo Chi,Jian Pu
Developing high-efficiency and cost-effective bifunctional electrocatalysts toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is an urgent issue for the oxygen-based electrochemical devices. Herein, an interface engineering concept has been proposed to achieve high-performance Ag–PBSC (Ag–PrBa 0.5 Sr 0.5 Co 2 O 5+δ ) heterostructure nanofibers catalyst. Benefiting from the significant ligand action and interparticle cooperation of exsolved Ag NPs and PBSC double perovskite, ORR/OER catalytic kinetics have been successfully boosted. In details, the PBSC double perovskite possessing abundant oxygen vacancies can provide oxygen channels and facilitate the transfer of electrons and oxygen. The embedded Ag NPs can deliver superior catalytic durability for the heterostructure interface. As expected, the as-synthesized Ag-PBSC heterostructure catalyst performs a favorable electrochemical performance in the oxygen-based applications. In alkaline media, the catalyst exhibits an excellent activity for ORR ( E onset : 0.88 V vs. RHE and E 1/2 : 0.72 V vs. RHE) and OER (1.67 V at 10 mA cm –2 ). When adopting the Ag–PBSC heterostructure catalyst in LOBs, the corresponding battery provides an outperforming capacity performance (13 000 mAh g –1 ), low discharge–charge polarization (1.37 V), and considerable cycling performance (128 cycles at the restricted capacity of 3 000 mAh g –1 and 400 mA g –1 ). Apparently, the work described here confirms that the interface engineering of perovskites can open up opportunities to develop highly active and durable heterostructure electrocatalysts for multitudinous oxygen-based electrochemical applications.
研究领域:
材料科学
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电化学
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能源存储与转换
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
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2021
·Vol. 5
·期 4
·1095-1102
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IF 6.367
Fen Li,Jinxia Li,Lihui Zhou,Sheng Dai
Metal–organic frameworks (MOFs) have recently emerged as one of the most promising electrocatalysts for oxygen evolution reaction (OER) due to their abundant metal sites and porous structures. However, the limited modulation of the single-metal sites of MOF-based catalysts restricts further promotion of their catalytic performance. In this work, we have developed a composite Co–Fe-based MOF catalyst based on Co–BDC (1,4-benzenedicarboxylate) and Fe–BDC, which modulated the electronic structure via the construction of the heterogeneous interfaces of Co–BDC and Fe–BDC. Enhanced OER performance was achieved in the composite Co–Fe–BDC catalyst, far more exceeding that of the counterpart Co–BDC or Fe–BDC. In addition, it was found that additional ultrasonic treatment effectively facilitated the dispersion of Fe–BDC on Co–BDC, as compared to the composited MOF obtained via physical mixture or magnetic stirring. The composite Co–Fe–BDC catalyst prepared via the ultrasonic-assisted one-pot synthesis exhibited an overpotential of 295 mV at a current density of 10 mA cm−2, which was even superior to that of the commercial RuO2 catalyst, while holding a lower cost and excellent stability. Insights gained in this study may shed new lights on heterogeneous interfaces and composition strategy of MOF-based electrochemical catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
ACS Catalysis
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2025
·
IF 13.1
Tengjia Ni,Dewei Zhang,Kaiyu Ji,Xianbiao Hou,Jian Zhou,Canhui Zhang,Lei Chu,Huanlei Wang,Shenghong Ju,Heqing Jiang,Minghua Huang
Understanding the intricate relationship between dynamic active site evolution and the pathway-selective oxygen evolution reaction (OER) is essential, yet it remains elusive. Herein, molecular-level integration of Ni-BDC (BDC = 1,4-benzenedicarboxylic acid) and Co-BPDC (BPDC = 4,4′-biphenyldicarboxylic acid) on Ni foam (NF) affords a self-adaptive bimetallic metal–organic framework (MOF)-on-MOF platform that enables dynamically responsive reconstruction into OER-active NiCoOOH/NF via real-time modulation of the coordination geometry at Ni–Co dual sites. Theoretical calculations and in situ spectroscopy uncover densely packed Ni–Co dual sites with shortened interatomic spacing in reconstructed NiCoOOH/NF, which facilitates the switching of the OER pathway from the adsorbate evolution mechanism (AEM) to the oxide pathway mechanism (OPM), thereby enabling spin-aligned O* intermediate formation and direct O–O* coupling for accelerated reaction kinetics. The resulting NiCoOOH/NF catalyst delivers an ultralow overpotential of 301 mV at 1 A cm–2 and maintains continuous operation beyond 1000 h. Upon integration into anion exchange membrane water electrolyzers (AEMWEs), it sustains a cell voltage of 1.77 V at 1 A cm–2 for durations exceeding 240 h. This work highlights a distinctive perspective on the fundamental mechanistic understanding of reconstructed catalysts.
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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能量存储与转换
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纳米材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Lu Yan,Liu Qingcui,Pang Xinxin,Tang Chenyang,Yan Zihan,Peng Banghua,Yu Feng
Ultrathin two-dimensional (2D) metal–organic framework (MOF) materials have become a research hotspot due to their ultra-large specific surface area and efficient charge transport, but their controllable preparation is still challenging. In this study, using molybdate anion, a small molecular modulation strategy is offered to precisely modulate the structure of cobalt-imidazolium MOF by liquid-phase reaction to successfully obtain ultrathin 2D MoCo-MOF shreds. High-valence molybdenum modulates the electronic structure and oxidation state of cobalt in MOFs, which in turn influences the growth of crystalline and morphology, leading to ultrathin MoCo-MOF structure. Synergism for molybdenum and cobalt in MoCo-MOF significantly enhanced the electrocatalytic activity of oxygen evolution reaction (OER) in 1M KOH. Meanwhile, the material also exhibited excellent uric acid (UA) detection performance with high sensitivity and wide detection range (4–800 μM). Our study verifies the effectiveness of oxometallate anion for structural modulation, provides a new way for material morphology modulation, and develops the potential of ultrathin 2D MoCo-MOF shreds for water electrolysis and UA detection.
研究领域:
材料科学
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电化学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
·
IF 5.4
Qing Chen,Ling Shi,Guiping Xu,Maocong Hu,Mao Peng,Zhenhua Yao
The development of low-cost and efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of importance for the commercialization of green and sustainable energy conversion devices. In this work, noble metal-free XFeCoNiCu (X = Cr, Mg, and Mn) high entropy alloys were prepared with a facile pyrolytic reduction approach while the structure and composition were characterized by XRD, ICP-OES, TEM, HRTEM, and XPS. The prepared quinary alloys demonstrated excellent activity and stability for both ORR and OER, which was even superior to that of commercial Pt/C and RuO₂. Moreover, all three catalysts exhibited considerable potential for bifunctional catalysis, with a ΔE gap of 0.659 V for CrFeCoNiCu, a ΔE gap of 0.692 V for MnFeCoNiCu, and a ΔE gap of 0.727 V for MgFeCoNiCu, which was much better than that of the Pt/C+RuO 2 combination (0.723 V). The superior performance was further revealed by Density Functional Theory (DFT) calculations with projection density of states (PDOS) and free energy change. The strategy proposed in this study provides an economical approach to design and develop bifunctional electrocatalysts with exceptional performance.
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
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Zhen-Long Wang,Ke-An Wang,Xuechun Xiao,Hai-Bin Zhu
Amorphous and crystalline catalysts both have their own advantages to reduce the overpotential of OER. However, there is limited research on the relationship between the OER catalytic performance and the crystallinity degree. Herein, this key issue was explored by preparing FeW oxides with varying degrees of crystallinity. DFT combined with practical experimental results indicate that the change in crystalline state not only affects the electronic interactions in Fe-W-O but also the M-O bond lengths, both influencing the spin state of FeW oxides. At the critical temperature of amorphous-to-crystalline transition, a low-spin state of Fe in FeWO-450 is found to optimize the adsorption of intermediates during OER. FeWO-450 exhibits even better performance than commercial noble metal catalysts and numerous catalysts reported in the literature. This work showcases the effect of crystallinity of metal oxides on electron spin and offer a guidance how to improve OER properties by altering the electron spin states.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122504
·
IF 7.5
Li Wu,Ziheng Bian,Jiaming Zhao,Yaqi Yang,Lili Guan,Yarong Huang,Xiwen Song
High–entropy oxide (HEO) are highly efficient electrocatalysts for the oxygen evolution reaction (OER), meeting the criteria for low cost, high activity, and long–term stability. This enhanced efficiency originates from their multicomponent composition and the synergistic interactions among the constituent elements. However, their inherent low conductivity and the lack of effective synthesis methods remain challenges. In this study, highly dispersed nanoscale spinel–type oxides (Fe 0.2 Co 0.2 Ni 0.2 Mn 0.2 Cr 0.2 ) 3 O 4 /CC, were prepared on carbon cloth (CC) through rapid one–step electrodeposition at room temperature, combined with Joule heating (JH), abbreviated as JH-HEO/CC. The introduction of abundant oxygen vacancies by JH's 'instantaneous–non–equilibrium' characteristic enhances ionic conductivity and optimizes reaction pathways. Thanks to these defects, the unique 'cocktail' effect allows these HEO to deliver a current density of 10 mA·cm −2 at an overpotential of 282 mV, while demonstrating excellent stability. This study establishes effective synthetic and modification strategies for high-performance OER electrocatalysts.
✓ 已验证
DOI
高影响因子
CARBON
·
2020
·
IF 8.821
Xingwei Zhou,Xin Liu,Jiahao Zhang,Cai Zhang,Seung Jo Yoo,Jin-Gyu Kim,Xianyu Chu,Chao Song,Peng Wang,Zhenzhen Zhao,Dabing Li,Wei Zhang,Weitao Zheng
Preventing agglomeration and corrosion of metal electrocatalysts at nanoscale is crucial for electrochemical energy conversion, such as fuel cell and overall water splitting , where all the oxygen evolution reaction (OER), hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) are the core. Herein, an effective strategy is developed for preparing multifunctional self-supporting electrocatalysts with uniformly distributed cobalt nanoparticles and clusters. Benefiting from good electrical conductivity and multiple active sites, the trifunctional self-supporting catalyst free from stacking and aggregating exhibits excellent OER and HER activities with an overpotential of 270 and 110 mV to obtain a current density of 10 mA cm −2 in alkaline media . The ORR performance was tested in 0.1 M KOH solution with a half-wave potential of ∼0.80 V and a limiting current density of ∼ −4.8 mA cm −2 . Our finding provides an opportunity for the rational design of multifunctional and highly-efficient self-supporting electrocatalysts towards the integration of electrochemical energy conversion.
研究领域:
材料科学
·
电化学能源转换
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）