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Transition metal-nitrogen-carbon (M-N-C) materials have been the focus of scientists’ efforts to address the rising need for earth-abundant materials solutions for energy technology and decarbonization of the economy. They are viewed as one of the most promising candidates to replace platinum group metal (PGM) catalysts in the fuel cell and energy conversion fields, including the application of oxygen reduction reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction. In the effort to improve M-N-C materials properties and achieve atomic dispersity of the transition metal in the carbonaceous matrix, a re-pyrolysis process has been proposed. This secondary heat treatment process of already obtained primary pyrolysis-derived M-N-C materials has been widely reported to substantially improve the electrochemical performance and operational stability of the catalysts. Here, we report a systematic investigation of this process used on samples of templated M-N-C catalysts to obtain state-of-the-art catalysts via in situ heating X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy (STEM), energy-dispersive X-ray spectroscopy (EDS), electron energy loss spectroscopy (EELS), X-ray diffraction (XRD), and X-ray computed tomography (CT) characterization methods. It is found that the re-pyrolysis of M-N-C materials could result in the partial amorphization of the carbonaceous substrate. It causes the rearrangement and transformation of multitudinous N moieties, leading to optimization of their morphological display and association with atomically dispersed transition metal dopants. Ultimately, the re-pyrolysis results in an increase in uniformity of the active Fe-Nx sites distribution without the formation of nano-crystalline phases (metallic or carbide) and with overall preservation of the morphology of the carbonaceous framework achieved during the first formative pyrolysis step of the templated synthesis. These observations provide confirmation that empirically established re-pyrolysis is recommended to be used on all M-N-C materials despite the different synthesis routes to obtain a practical advanced catalytic material. 相似文献
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Callistus Nonso Ude Dominic Okechukwu Onukwuli Jonah Chukwudi Umeuzuegbu Chinemelum Chukwujekwu Chukwuka 《化学工程与技术》2021,44(1):65-76
The heterogeneous catalysis of transesterification of gmelina seed oil to biodiesel is evaluated. The oil was extracted from the seeds with n‐hexane by solvent extraction and characterized to determine its physiochemical properties. Response surface methodology was applied to optimize the effect of process variables on the biodiesel yield. The base‐activated clay catalyst performed as montmorillonite clay with the characteristic property of a Brønsted acid. It has an improved surface area after activation that enhanced its catalytic activity on transesterification reaction. Under optimal conditions, the biodiesel yield was 70.1 %, thus demonstrating that the model predicted well the biodiesel production. 相似文献
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Shunsuke Kato Prof. Akira Onoda Naomasa Taniguchi Prof. Ulrich Schwaneberg Prof. Takashi Hayashi 《Chembiochem : a European journal of chemical biology》2021,22(4):679-685
Directed evolution of Cp*RhIII-linked nitrobindin (NB), a biohybrid catalyst, was performed based on an in vitro screening approach. A key aspect of this effort was the establishment of a high-throughput screening (HTS) platform that involves an affinity purification step employing a starch-agarose resin for a maltose binding protein (MBP) tag. The HTS platform enables efficient preparation of the purified MBP-tagged biohybrid catalysts in a 96-well format and eliminates background influence of the host E. coli cells. Three rounds of directed evolution and screening of more than 4000 clones yielded a Cp*RhIII-linked NB(T98H/L100K/K127E) variant with a 4.9-fold enhanced activity for the cycloaddition of acetophenone oximes with alkynes. It is confirmed that this HTS platform for directed evolution provides an efficient strategy for generating highly active biohybrid catalysts incorporating a synthetic metal cofactor. 相似文献
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Xiaoqin Yang Huy Q. Ta Huimin Hu Shuyuan Liu Yu Liu Alicja Bachmatiuk Jinping Luo Lijun Liu Jin-Ho Choi Mark H. Rummeli 《Advanced functional materials》2021,31(38):2104340
In this study, in situ transmission electron microscopy is performed to study the interaction between single (monomer) and paired (dimer) Sn atoms at graphene edges. The results reveal that a single Sn atom can catalyze both the growth and etching of graphene by the addition and removal of C atoms respectively. Additionally, the frequencies of the energetically favorable configurations of an Sn atom at a graphene edge, calculated using density functional theory calculations, are compared with experimental observations and are found to be in good agreement. The remarkable dynamic processes of binary atoms (dimers) are also investigated and is the first such study to the best of the knowledge. Dimer diffusion along the graphene edges depends on the graphene edge termination. Atom pairs (dimers) involving an armchair configuration tend to diffuse with a synchronized shuffling (step-wise shift) action, while dimer diffusion at zigzag edge terminations show a strong propensity to collapse the dimer with each atom diffusing in opposite directions (monomer formation). Moreover, the data reveals the role of C feedstock availability on the choice a single Sn atom makes in terms of graphene growth or etching. This study advances the understanding single atom catalytic activity at graphene edges. 相似文献
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Non-oxidative dehydroaromatization is arguably the most promising process for the direct upgrading of cheap and abundant methane to liquid hydrocarbons. This reaction has not been commercialized yet because of the suboptimal activity and swift deactivation of benchmark Mo-zeolite catalysts. This progress report represents an elaboration on the recent developments in understanding of zeolite-based catalytic materials for high-temperature non-oxidative dehydroaromatization of methane. It is specifically focused on recent studies, relevant to the materials chemistry and elucidating i) the structure of active species in working catalysts; ii) the complex molecular pathways underlying the mechanism of selective conversion of methane to benzene; iii) structure, evolution and role of coke species; and iv) process intensification strategies to improve the deactivation resistance and overall performance of the catalysts. Finally, unsolved challenges in this field of research are outlined and an outlook is provided on promising directions toward improving the activity, stability, and selectivity of methane dehydroaromatization catalysts. 相似文献
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采用酸处理方法对CoPd/TiO2催化剂进行改性,并将酸改性催化剂用于温和条件下CH4-CO2梯阶转化直接合成C2含氧化合物(乙酸和乙醇)的反应。在150~300℃考察了浸酸方式和不同种类酸处理对催化剂活性和选择性的影响。采用X射线衍射(XRD)、X射线光电子能谱(XPS)、NH3程序升温脱附(NH3-TPD)和N2吸附对催化剂进行了表征。结果表明,酸改性明显提高了CoPd/TiO2上C2含氧化合物的生成速率和选择性。浸酸方式对催化剂性能和结构有显著影响,先用酸浸渍载体然后再浸渍活性金属所得催化剂具有更高的活性。在H3PO4、HNO3和HCl中,H3PO4浸渍的催化剂活性最佳,在150℃时C2含氧化合物(乙酸和乙醇)的生成速率为3365 μg/(g·h),选择性达到91%。 相似文献
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通过制备不同晶相结构〔单斜相(m-ZrO_2)、四方相(t-ZrO_2)和无定型(a-ZrO_2)〕ZrO_2载体,再通过沉积沉淀法制得Cu/m-ZrO_2、Cu/t-ZrO_2和Cu/a-ZrO_2催化剂,分别用于催化二乙醇胺脱氢合成亚氨基二乙酸反应。采用XRD、氮气物理吸附脱附、XPS、H_2-TPR、CO_2-TPD对催化剂的结构进行了表征。结果表明,Cu/m-ZrO_2催化剂界面更加有利于Cu~+/Cu~0稳定存在,具有更多的碱性位点,且抗氧化性较好。在二乙醇胺脱氢反应中,Cu/m-ZrO_2催化剂性能最好,反应时间为2.5 h,亚氨基二乙酸收率为97.64%。 相似文献