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Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

《化学科学与工程前沿（英文）》 doi: 10.1007/s11705-022-2247-y

摘要： Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe₂Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe₂Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO₂(110) catalysts. The analysis of the potential gap of Fe₂M clusters indicates that Fe₂Mn, Fe₂Co, and Fe₂Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe₂Mn and Fe₂Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe₂M–PCN–Fe₂M is explored. Compared with Fe₂Mn–PCN–Fe₂Mn, Fe₂Co–PCN–Fe₂Co, and isolated Fe₂M clusters, the mixed-metal Fe₂Co–PCN–Fe₂Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe₂Co–PCN–Fe₂Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词： bimetallic metal–organic frameworks bifunctional electrocatalyst density functional theory oxygen reduction reaction oxygen evolution reaction

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A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

《能源前沿（英文）》 2017年第11卷第3期页码 268-285 doi: 10.1007/s11708-017-0466-6

摘要： Development of active and durable electrocatalyst for oxygen reduction reaction (ORR) remains one challenge for the polymer electrolyte membrane fuel cell (PEMFC) technology. Pt-based nanomaterials show the greatest promise as electrocatalyst for this reaction among all current catalytic structures. This review focuses on Pt-based ORR catalyst material development and covers the past achievements, current research status and perspectives in this research field. In particular, several important categories of Pt-based catalytic structures and the research advances are summarized. Key factors affecting the catalyst activity and durability are discussed. An outlook of future research direction of ORR catalyst research is provided.

关键词： oxygen reduction reaction (ORR) electrocatalysis platinum catalyst activity durability

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Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

《化学科学与工程前沿（英文）》 2018年第12卷第4期页码 790-797 doi: 10.1007/s11705-018-1706-y

摘要： A noble-metal-free catalyst based on both Mn O and MnO was prepared by using the dielectric barrier discharge technique at moderate temperature. The prepared catalyst shows a higher electrocatalytic activity towards the oxygen reduction reaction than the catalyst prepared by using the traditional calcination process. The enhanced activity could be due to the coexistence of manganese ions with different valences, the higher oxygen adsorption capacity, and the suppressed aggregation of the catalyst nanoparticles at moderate temperature. The present work would open a new way to prepare low-cost and noble-metal-free catalysts at moderate temperature for more efficient electrocatalysis.

关键词： oxygen reduction reaction manganese oxides mixed valences of manganese oxygen adsorption dielectric barrier discharge

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Pt-Ni nanourchins as electrocatalysts for oxygen reduction reaction

Qiaowan CHANG, Yuan XU, Shangqian ZHU, Fei XIAO, Minhua SHAO

《能源前沿（英文）》 2017年第11卷第3期页码 254-259 doi: 10.1007/s11708-017-0493-3

摘要： Pt-Ni bimetallic alloys with various nanostructures have shown excellent activity toward oxygen reduction reaction (ORR). The ORR activity is highly dependent on the structure of the catalyst. In this paper, Pt-Ni nanourchins were synthesized with an average size of 50 nm consisting of 10–20 nanorods and nanooctahedra by adjusting the synthesis condition. The formation of Pt-Ni nanourchins is mainly dependent on the adding order of solvents (benzyl ether, oleylamine and oleic acid). Pt-Ni nanourchins present a reasonable high ORR activity (0.81 A/mg at 0.9 V).

关键词： Pt-Ni alloys nanourchins oxygen reduction reaction shape control fuel cells

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Enhanced electrocatalytic performance of ultrathin PtNi alloy nanowires for oxygen reduction reaction

Hongjie ZHANG, Yachao ZENG, Longsheng CAO, Limeng YANG, Dahui FANG, Baolian YI, Zhigang SHAO

《能源前沿（英文）》 2017年第11卷第3期页码 260-267 doi: 10.1007/s11708-017-0499-x

摘要： In this paper, ultrathin Pt nanowires (Pt NWs) and PtNi alloy nanowires (PtNi NWs) supported on carbon were synthesized as electrocatalysts for oxygen reduction reaction (ORR). Pt and PtNi NWs catalysts composed of interconnected nanoparticles were prepared by using a soft template method with CTAB as the surface active agent. The physical characterization and electrocatalytic performance of Pt NWs and PtNi NWs catalysts for ORR were investigated and the results were compared with the commercial Pt/C catalyst. The atomic ratio of Pt and Ni in PtNi alloy was approximately 3 to 1. The results show that after alloying with Ni, the binding energy of Pt shifts to higher values, indicating the change of its electronic structure, and that Pt Ni NWs catalyst has a significantly higher electrocatalytic activity and good stability for ORR as compared to Pt NWs and even Pt/C catalyst. The enhanced electrocatalytic activity of Pt Ni NWs catalyst is mainly resulted from the downshifted-band center of Pt caused by the interaction between Pt and Ni in the alloy, which facilitates the desorption of oxygen containing species (O or OH ) and the release of active sites.

关键词： PtNi alloy nanowires oxygen reduction reaction enhanced activity good stability

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Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

《化学科学与工程前沿（英文）》 2015年第9卷第3期页码 280-294 doi: 10.1007/s11705-015-1524-4

摘要： Developing metal-free, carbon-based catalysts to replace platinum-based catalysts for oxygen reduction reactions (ORRs) is an emerging area of research. In recent years, different carbon structures including carbon doped with IIIA-VIIA heteroatoms (C−M site-based, where M represents the doped heteroatom) and polynitrogen (PN) compounds encapsulated in carbon nanotubes (CNTs) (N−N site-based) have been synthesized. Compared to metallic catalysts, these materials are highly active, stable, inexpensive, and environmentally friendly. This review discusses the development of these materials, their ORR performances and the mechanisms for how the incorporation of heteroatoms enhances the ORR activity. Strategies for tailoring the structures of the carbon substrates to improve ORR performance are also discussed. Future studies in this area will need to include optimizing synthetic strategies to control the type, amount and distribution of the incorporated heteroatoms, as well as better understanding the ORR mechanisms in these catalysts.

关键词： oxygen reduction reaction electrocatalysis metal-free carbon-based polynitrogen

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Highly active and durable Pd-Cu catalysts for oxygen reduction in alkaline exchange membrane fuel cells

Xiong PENG, Travis J. OMASTA, Justin M. ROLLER, William E. MUSTAIN

《能源前沿（英文）》 2017年第11卷第3期页码 299-309 doi: 10.1007/s11708-017-0495-1

摘要： A Pd-Cu catalyst, with primary B2-type phase, supported by VulcanXC-7R carbon was synthesized via a solvothermal method. The catalysts were physically and electrochemically characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and both cyclic and linear sweep voltammetry using a rotating disk electrode (RDE). During the RDE testing, the half-wave potential of the Pd-Cu/Vulcan catalyst was 50 mV higher compared to that of commercial Pt/C catalyst for the oxygen reduction reaction (ORR) in alkaline media. The Pd-Cu/Vulcan exhibited a specific activity of 1.27 mA/cm and a mass activity of 0.59 A/mg at 0.9 V, which were 4 and 3 times greater than that of the commercial Pt/C catalyst, respectively. The Pd-Cu/Vulcan catalyst also showed higher alkaline exchange membrane fuel cell (AEMFC) performance, with operating power densities of 1100 MW/cm operating on H /O and 700 MW/cm operating on H /Air (CO -free), which were markedly higher than those of the commercial Pt/C. The Pd-Cu/Vulcan catalyst also exhibited high stability during a short-term, AEMFC durability test, with only around 11% performance loss after 30 hours of operation, an improvement over most AEMFCs reported in the literature to date.

关键词： alkaline exchange membrane (AEM) fuel cell Pd-Cu oxygen reduction high performance water

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Reduction kinetics of SrFeO/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial

《化学科学与工程前沿（英文）》页码 1726-1734 doi: 10.1007/s11705-022-2188-5

摘要： Chemical looping reforming of methane is a novel and effective approach to convert methane to syngas, in which oxygen transfer is achieved by a redox material. Although lots of efforts have been made to develop high-performance redox materials, a few studies have focused on the redox kinetics. In this work, the kinetics of SrFeO_3−δ–CaO∙MnO nanocomposite reduction by methane was investigated both on a thermo-gravimetric analyzer and in a packed-bed microreactor. During the methane reduction, combustion occurs before the partial oxidation and there exists a transition between them. The weight loss due to combustion increases, but the transition region becomes less inconspicuous as the reduction temperature increased. The weight loss associated with the partial oxidation is much larger than that with combustion. The rate of weight loss related to the partial oxidation is well fitted by the Avrami–Erofeyev equation with n = 3 (A3 model) with an activation energy of 59.8 kJ∙mol^‒1. The rate law for the partial oxidation includes a solid conversion term whose expression is given by the A3 model and a methane pressure-dependent term represented by a power law. The partial oxidation is half order with respect to methane pressure. The proposed rate law could well predict the reduction kinetics; thus, it may be used to design and/or analyze a chemical looping reforming reactor.

关键词： chemical looping reforming SrFeO_3−δ/CaO·MnO nanocomposite reduction kinetics Avrami–Erofeyev model pressure-dependent term

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Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2022年第16卷第5期页码 812-821 doi: 10.1007/s11708-020-0669-0

摘要： The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N , accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

关键词： oxygen reduction reaction Fe-N-C active sites Fe addition second heat treatment

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Thermal annealing synthesis of double-shell truncated octahedral Pt-Ni alloys for oxygen reduction reaction

Xiashuang LUO, Yangge GUO, Hongru ZHOU, Huan REN, Shuiyun SHEN, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2020年第14卷第4期页码 767-777 doi: 10.1007/s11708-020-0667-2

摘要： Shape-controlled Pt-Ni alloys usually offer an exceptional electrocatalytic activity toward the oxygen reduction reaction (ORR) of polymer electrolyte membrane fuel cells (PEMFCs), whose tricks lie in well-designed structures and surface morphologies. In this paper, a novel synthesis of truncated octahedral PtNi alloy catalysts that consist of homogeneous Pt-Ni alloy cores enclosed by NiO-Pt double shells through thermally annealing defective heterogeneous PtNi alloys is reported. By tracking the evolution of both compositions and morphologies, the outward segregation of both PtO and NiO are first observed in Pt-Ni alloys. It is speculated that the diffusion of low-coordination atoms results in the formation of an energetically favorable truncated octahedron while the outward segregation of oxides leads to the formation of NiO-Pt double shells. It is very attractive that after gently removing the NiO outer shell, the dealloyed truncated octahedral core-shell structure demonstrates a greatly enhanced ORR activity. The as-obtained truncated octahedral Pt Ni core-shell alloy presents a 3.4-folds mass-specific activity of that for unannealed sample, and its activity preserves 45.4% after 30000 potential cycles of accelerated degradation test (ADT). The peak power density of the dealloyed truncated octahedral Pt Ni core-shell alloy catalyst based membrane electrolyte assembly (MEA) reaches 679.8 mW/cm , increased by 138.4 mW/cm relative to that based on commercial Pt/C.

关键词： dealloyed Pt-Ni alloys truncated octahedron double-shell thermal annealing oxygen reduction reaction (ORR)

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Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygen

《化学科学与工程前沿（英文）》 2021年第15卷第6期页码 1550-1560 doi: 10.1007/s11705-021-2104-4

摘要： The low cost and highly efficient construction of electrocatalysts has attracted significant attention owing to the use of clean and sustainable energy technologies. In this work, cobalt nanoparticle decorated N-doped carbons (Co@NC) are synthesized by the pyrolysis of a cobalt covalent organic framework under an inert atmosphere. The Co@NC demonstrates improved electrocatalytic capabilities compared to N-doped carbon without the addition of Co nanoparticles, indicating the important role of cobalt. The well-dispersed active sites (Co-N_x) and the synergistic effect between the carbon matrix and Co nanoparticles greatly enhance the electrocatalytic activity for the oxygen reduction reaction. In addition, the Co content has a significant effect on the catalytic activity. The resulting Co@NC-0.86 exhibits a superb electrocatalytic activity for the oxygen reduction reaction in an alkaline electrolyte in terms of the onset potential (0.90 V), half-wave potential (0.80 V) and the limiting current density (4.84 mA·cm^–2), and a high selectivity, as well as a strong methanol tolerance and superior durability, these results are comparable to those of the Pt/C catalyst. Furthermore, the superior bifunctional activity of Co@NC-0.86 was also confirmed in a home-built Zn-air battery, signifying the possibility for application in electrode materials and in current energy conversion and storage devices.

关键词： cobalt embedment N-doped carbons covalent organic framework oxygen reduction Zn-air battery

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Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

《化学科学与工程前沿（英文）》 2021年第15卷第5期页码 1206-1216 doi: 10.1007/s11705-020-2017-7

摘要： In this work, the detailed oxygen reduction reaction (ORR) catalytic performance of M-N O (M= Fe, Co, and Ni; = 1–4) has been explored via the detailed density functional theory method. The results suggest that the formation energy of M-N O shows a good linear relationship with the number of doped O atoms. The adsorption manner of O on M-N O changed from end-on ( = 1 and 2) to side-on ( = 3 and 4), and the adsorption strength gradually increased. Based on the results for binding strength of ORR intermediates and the Gibbs free energy of ORR steps on the studied catalysts, we screened out two highly active ORR catalysts, namely Co-N O and Ni-N O , which possess very small overpotentials of 0.27 and 0.32 V, respectively. Such activities are higher than the precious Pt catalyst. Electronic structure analysis reveals one of the reasons for the higher activity of Co-N O and Ni-N O is that they have small energy gaps and moderate highest occupied molecular orbital energy levels. Furthermore, the results of the density of states reveal that the O doping can improve the electronic structure of the original catalyst to tune the adsorption of the ORR intermediates.

关键词： M-N-C catalyst oxygen doping oxygen reduction reaction catalytic activity density functional theory

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Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

《环境科学与工程前沿（英文）》 2015年第9卷第6期页码 1130-1138 doi: 10.1007/s11783-015-0821-y

摘要： Chemical looping combustion is a promising technology for energy conversion due to its low-carbon, high-efficiency, and environmental-friendly feature. A vital issue for CLC process is the development of oxygen carrier, since it must have sufficient reactivity. The mechanism and kinetics of CO reduction on iron-based oxygen carriers namely pure Fe O and Fe O supported by alumina (Fe O /Al O ) were investigated using thermo-gravimetric analysis. Fe O /Al O showed better reactivity over bare Fe O toward CO reduction. This was well supported by the observed higher rate constant for Fe O /Al O over pure Fe O with respective activation energy of 41.1±2.0 and 33.3±0.8 kJ·mol . The proposed models were compared via statistical approach comprising Akaike information criterion with correction coupled with F-test. The phase-boundary reaction and diffusion control models approximated to 95% confidence level along with scanning electron microscopy results; revealed the promising reduction reactions of pure Fe O and Fe O /Al O . The boosting recital of iron-based oxygen carrier support toward efficient chemical looping combustion could be explained accurately through the present study.

关键词： chemical looping combustion iron-based oxygen carriers reduction kinetics carbon monoxide statistics

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In situ DRIFTS study of photocatalytic CO 2 reduction under UV irradiation

Jeffrey C. S. WU, Chao-Wei HUANG,

《化学科学与工程前沿（英文）》 2010年第4卷第2期页码 120-126 doi: 10.1007/s11705-009-0232-3

摘要： Photocatalytic reduction of CO on TiO and Cu/TiO photocatalysts was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) under UV irradiation. The photocatalysts were prepared by sol-gel method via controlled hydrolysis of titanium (IV) butoxide. Copper precursor was loaded onto TiO during sol-gel procedure. A large amount of adsorbed HO and surface OH groups was detected at 25°C on the TiO photocatalyst after being treated at 500°C under air stream. Carbonate and bicarbonate were formed rapidly due to the reaction of CO with oxygen-vacancy and OH groups, respectively, on TiO surface upon CO adsorption. The IR spectra indicated that, under UV irradiation, gas-phase CO further combined with oxygen-vacancy and OH groups to produce more carbonate or bicarbonate. The weak signals of reaction intermediates were found on the IR spectra, which were due to the slow photocatalytic CO reduction on photocatalysts. Photogenerated electrons merge with H ions to form H atoms, which progressively reduce CO to form formic acid, dioxymethylene, formaldehyde and methoxy as observed in the IR spectra. The well-dispersed Cu, acting as the active site significantly increases the amount of formaldehyde and dioxymethylene, thus promotes the photoactivity of CO reduction on Cu/TiO. A possible mechanism of the photocatalytic CO reduction is proposed based on these intermediates and products on the photocatalysts.

关键词： irradiation oxygen-vacancy Photocatalytic reduction Carbonate butoxide

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Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer boosting oxygen

《化学科学与工程前沿（英文）》 doi: 10.1007/s11705-022-2232-5

摘要： Fe–N_x nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–N_x nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–N_x nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e^– transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm^–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

关键词： Fe–N_x nanoparticles hypersaline-confinement conversion floret-like carbon covalent triazine polymers oxygen reduction reaction

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标题作者时间类型操作

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

期刊论文

A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

期刊论文

Multivalent manganese oxides with high electrocatalytic activity for oxygen reduction reaction

Xiangfeng Peng, Zhenhai Wang, Zhao Wang, Yunxiang Pan

期刊论文

Pt-Ni nanourchins as electrocatalysts for oxygen reduction reaction

Qiaowan CHANG, Yuan XU, Shangqian ZHU, Fei XIAO, Minhua SHAO

期刊论文

Enhanced electrocatalytic performance of ultrathin PtNi alloy nanowires for oxygen reduction reaction

Hongjie ZHANG, Yachao ZENG, Longsheng CAO, Limeng YANG, Dahui FANG, Baolian YI, Zhigang SHAO

期刊论文

Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

期刊论文

Highly active and durable Pd-Cu catalysts for oxygen reduction in alkaline exchange membrane fuel cells

Xiong PENG, Travis J. OMASTA, Justin M. ROLLER, William E. MUSTAIN

期刊论文

Reduction kinetics of SrFeO/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial

期刊论文

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

期刊论文

Thermal annealing synthesis of double-shell truncated octahedral Pt-Ni alloys for oxygen reduction reaction

Xiashuang LUO, Yangge GUO, Hongru ZHOU, Huan REN, Shuiyun SHEN, Guanghua WEI, Junliang ZHANG

期刊论文

Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygen

期刊论文

Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

期刊论文

Performance and kinetics of iron-based oxygen carriers reduced by carbon monoxide for chemical looping

Xiuning HUA,Wei WANG,Feng WANG

期刊论文

In situ DRIFTS study of photocatalytic CO 2 reduction under UV irradiation

Jeffrey C. S. WU, Chao-Wei HUANG,

期刊论文

Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer boosting oxygen

期刊论文

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