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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）》 2023年 第17卷 第5期   页码 570-580 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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Highly efficient and active Co–N–C catalysts for oxygen reduction and Zn–air batteries

《能源前沿（英文）》 doi: 10.1007/s11708-024-0928-6

摘要： In this study, the Lewis doping approach of polyaniline (PANI) was employed to fabricate cobait–nitrogen–carbon (Co–N–C) oxygen electrocatalysts for Zn–air batteries, aiming to enhance the active spots of Co–N–C. This resulting Co–N–C catalysts exhibited well-defined nanofiber networks, and the Brunauer-Emmett-Teller (BET) analysis confirmed their substantial specific surface area. Electrochemical experiments demonstrated that the Co–N–C catalysts achieved the half-wave potential (vs. RHE) of 0.85 V in alkaline medium, overcoming Pt/C and iron–nitrogen–carbon (Fe–N–C) counterparts in extended cycle testing with only a 25 mV change in a half-wave potential after 5000 cycles. Remarkably, the highest power density measured in the zinc (Zn)-air battery reached 227 mW/cm2, a significant improvement over the performance of 101 mW/cm2 of the platinum on activated carbon (Pt/C) catalyst. These findings highlight the advantageous stability enhancement associated with the utilization of Co in the Co–N–C catalysts.

关键词： oxygen reduction reaction (ORR)     oxygen evolution reaction (OER)     non-noble metal catalysts     Co–N–C catalysts     Zn–air battery    

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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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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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Strain engineering of Pt-based electrocatalysts for oxygen reaction reduction

《能源前沿（英文）》 2024年 第18卷 第2期   页码 241-262 doi: 10.1007/s11708-024-0932-x

摘要： Proton exchange membrane fuel cells (PEMFCs) are playing irreplaceable roles in the construction of the future sustainable energy system. However, the insufficient performance of platinum (Pt)-based electrocatalysts for oxygen reduction reaction (ORR) hinders the overall efficiency of PEMFCs. Engineering the surface strain of catalysts is considered an effective way to tune their electronic structures and therefore optimize catalytic behavior. In this paper, insights into strain engineering for improving Pt-based catalysts toward ORR are elaborated in detail. First, recent advances in understanding the strain effects on ORR catalysts are comprehensively discussed. Then, strain engineering methodologies for adjusting Pt-based catalysts are comprehensively discussed. Finally, further information on the various challenges and potential prospects for strain modulation of Pt-based catalysts is provided.

关键词： strain engineering     Pt-based catalysts     oxygen reduction reaction (ORR)     catalytic performance     proton exchange membrane fuel cells (PEMFCs)    

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Recent advances in morphology control of platinum catalysts toward oxygen reduction reaction

《能源前沿（英文）》 2024年 第18卷 第3期   页码 330-355 doi: 10.1007/s11708-024-0929-5

摘要： Exploring advanced platinum (Pt)-based electrocatalysts is vital for the widespread implementation of proton exchange membrane fuel cells (PEMFCs). Morphology control represents an effective strategy to optimize the behavior of Pt catalysts. In this work, an attempt is made to comprehensively review the effect of morphology control on the catalytic behavior of catalysts in the oxygen reduction reaction (ORR). First, the fundamental physicochemical changes behind morphology control, including exposing more active sites, generating appropriate lattice strains, and forming different crystalline surfaces, are highlighted. Then, recently developed strategies for tuning the morphologies of electrocatalysts, including core-shell structures, hollow structures, nanocages, nanowires, and nanosheets, are comprehensively summarized. Finally, an outlook on the future development of morphology control of Pt catalysts is presented, including rational design strategies, advanced in situ characterization techniques, novel artificial intelligence, and mechanical learning. This work is intended to provide valuable insights into designing the morphology and technological innovation of efficient redox electrocatalysts in fuel cells.

关键词： morphology     platinum catalysts     electrocatalysis     ORR     PEMFC    

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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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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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Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for proton

《能源前沿（英文）》 2024年 第18卷 第2期   页码 206-222 doi: 10.1007/s11708-023-0907-3

摘要： Platinum (Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). However, their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading reduction. Based on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts, Pt single-atom catalysts (Pt SACs) as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this paper. The design thoughts and synthesis of various isolated, alloyed, and nanoparticle-contained Pt SACs are summarized. The single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the catalysts. To advance further research and development of Pt SACs for viable implementation in PEMFCs, various technical challenges and several potential research directions are outlined.

关键词： oxygen reduction electrocatalysis     Pt single-atom catalysts     conventional Pt-based catalysts     design thoughts and synthesis     metal-support interactions    

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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）》 2022年 第16卷 第12期   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 SrFeO3−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     SrFeO3−δ/CaO·MnO nanocomposite     reduction kinetics     Avrami–Erofeyev model     pressure-dependent term    

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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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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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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

Highly efficient and active Co–N–C catalysts for oxygen reduction and Zn–air batteries

期刊论文

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

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

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

Strain engineering of Pt-based electrocatalysts for oxygen reaction reduction

期刊论文

Recent advances in morphology control of platinum catalysts toward oxygen reduction reaction

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

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

Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for proton

期刊论文

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

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

Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

期刊论文