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学者姓名：彭小波
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Abstract ：
The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory reaction performance owing to the low aqueous solubility of N-2 in aqueous solution, the high dissociation energy of N equivalent to N, and the unavoidable competing hydrogen evolution reaction (HER). Herein, a MIL-53(Fe)@TiO2 catalyst is designed and synthesized for highly efficient eNRR. Relative to simple MIL-53(Fe), MIL-53(Fe)@TiO(2 )achieves a 2-fold enhancement in the Faradaic efficiency (FE) with an improved ammonia yield rate by 76.5% at -0.1 V versus reversible hydrogen electrode (RHE). After four cycles of electrocatalysis, MIL-53(Fe)@TiO2 can maintain a good catalytic activity, while MIL-53(Fe) exhibits a significant decrease in the NH3 yield rate and FE by 79.8 and 82.3%, respectively. Benefiting from the synergetic effect between TiO2 and MIL-53(Fe) in the composites, Fe3+ ions can be greatly stabilized in MIL-53(Fe) during the eNRR process, which greatly hinders the catalyst deactivation caused by the electrochemical reduction of Fe3+ ions. Further, the charge transfer ability in the interface of composites can be improved, and thus, the eNRR activity is significantly boosted. These findings provide a promising insight into the preparation of efficient composite electrocatalysts.
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| GB/T 7714 | Sun, Zhuangzhi , Lin, Jiawei , Lu, Suwei et al. Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction [J]. | LANGMUIR , 2024 , 40 (10) : 5469-5478 . |
| MLA | Sun, Zhuangzhi et al. "Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction" . | LANGMUIR 40 . 10 (2024) : 5469-5478 . |
| APA | Sun, Zhuangzhi , Lin, Jiawei , Lu, Suwei , Li, Yuhang , Qi, Tingting , Peng, Xiaobo et al. Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction . | LANGMUIR , 2024 , 40 (10) , 5469-5478 . |
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As a sustainable and economical strategy, electrochemical nitrogen reduction reaction (eNRR) is a promising alternative of energy-intensive Haber-Bosch process to produce ammonia. Fabricating efficient catalysts for eNRR is still challenging due to the bottleneck of insufficient activity and low electron selectivity. Herein, phosphotungstic acid (PTA) as substrate to anchor cerium species on the 4-fold hollow site was prepared, which reaches high ammonia yield rates of 42 mu g h-1 mgcat-1 and Faradaic efficiencies of 9.2 % at-0.6 V versus reversible hydrogen electrode. Experiments and theoretical calculations reveal that the introduction of Ce species could significantly improve the electronic density of adjacent exposed W atoms, further boosting the effective adsorption and activation of N2 to form active *N2. Finally, the designed Ce-PTA catalysts show high electrocatalytic activity of N2 reduction into ammonia. This work highlights the important role of using PTA as substrate to prepare stable supported metal species for heterogeneous electrocatalysis.
Keyword ：
Ammonia synthesis Ammonia synthesis Ce species modification Ce species modification Electrocatalysis Electrocatalysis N2 reduction reaction N2 reduction reaction Phosphotungstic acid Phosphotungstic acid
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| GB/T 7714 | Liu, Dan , Yan, Hongping , Lin, Jiawei et al. Regulation of cerium species in Keggin structure of phosphotungstic acid for efficient nitrogen electroreduction to ammonia [J]. | CHEMICAL ENGINEERING SCIENCE , 2023 , 283 . |
| MLA | Liu, Dan et al. "Regulation of cerium species in Keggin structure of phosphotungstic acid for efficient nitrogen electroreduction to ammonia" . | CHEMICAL ENGINEERING SCIENCE 283 (2023) . |
| APA | Liu, Dan , Yan, Hongping , Lin, Jiawei , Lu, Suwei , Xie, Yaoqi , Peng, Xiaobo et al. Regulation of cerium species in Keggin structure of phosphotungstic acid for efficient nitrogen electroreduction to ammonia . | CHEMICAL ENGINEERING SCIENCE , 2023 , 283 . |
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本发明公开了一种介孔碳负载铜铁双金属催化剂及其制备方法与应用，以铜盐和铁盐为金属源，碱作为沉淀剂，通过分批次投料，利用水热共沉淀作用，制备得到铜铁双金属氧化物，与有序介孔碳混磨均匀后经H2还原得到介孔碳负载铜铁双金属催化剂，并将其用于电催化硝酸根还原合成氨反应中。本发明制得的介孔碳负载铜铁双金属催化剂具有双金属协同效应，能在催化剂上有效吸附活化硝酸根，并将其转化为氨，且介孔碳载体的存在使得催化剂具有较大的比表面积和良好的电导性，并且增强了催化剂的稳定性，使得催化剂具有良好的电催化硝酸根还原性能。本发明的制备方法简单便捷、能耗小、成本低，有较大的应用潜力。
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| GB/T 7714 | 刘福建 , 刘丽娟 , 梁诗景 et al. 一种介孔碳负载铜铁双金属催化剂及其制备方法与应用 : CN202210249491.8[P]. | 2022-03-14 00:00:00 . |
| MLA | 刘福建 et al. "一种介孔碳负载铜铁双金属催化剂及其制备方法与应用" : CN202210249491.8. | 2022-03-14 00:00:00 . |
| APA | 刘福建 , 刘丽娟 , 梁诗景 , 彭小波 , 江莉龙 . 一种介孔碳负载铜铁双金属催化剂及其制备方法与应用 : CN202210249491.8. | 2022-03-14 00:00:00 . |
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本发明公开了一种介孔炭球包裹的锆负载型催化剂的制备方法，以原硅酸四丙酯、原硅酸四乙酯、间苯二酚、甲醛为原料，采用模板法制备出介孔中空炭球载体；随后以磷钨酸、硫酸锆为原料，通过分批次投料，在温和条件下加热搅拌制备得到锆负载磷钨酸催化剂；再通过浸渍法将锆负载磷钨酸催化剂固载化到介孔中空炭球的多级孔道中，首次开发出高活性、高稳定性的介孔炭球包裹的锆负载磷钨酸电催化剂；本发明制备的电催化剂具有强氮气活化能力，可以有效抑制析氢副反应，具备了优秀的电催化合成氨活性和选择性，同时在空间限域的作用下展现出良好的化学结构和性能稳定性。
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| GB/T 7714 | 梁诗景 , 廖婉茹 , 江莉龙 et al. 一种介孔炭球包裹的锆负载型催化剂的制备方法及其应用 : CN202210333046.X[P]. | 2022-03-31 00:00:00 . |
| MLA | 梁诗景 et al. "一种介孔炭球包裹的锆负载型催化剂的制备方法及其应用" : CN202210333046.X. | 2022-03-31 00:00:00 . |
| APA | 梁诗景 , 廖婉茹 , 江莉龙 , 彭小波 . 一种介孔炭球包裹的锆负载型催化剂的制备方法及其应用 : CN202210333046.X. | 2022-03-31 00:00:00 . |
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The development of low-cost nickel-based catalysts for direct and selective hydrogenation of 2-butyne-1,4-diol (BYD) to butane-1,4-diol (BAD) under mild conditions is an important and attractive target both in fundamental research and industrialization but remains a formidable challenge. The primary industrial production method for BAD synthesis is a two-step reaction route, which suffers from complicated catalysis conditions and high equipment costs. Herein, we develop a high-performance catalyst via a facile alcohol-treated strategy for highly selective BAD synthesis at moderate operation conditions. The as-synthesized NA-80E catalyst exhibits outstanding BAD selectivity of 98.82 % and BYD conversion of 100 % at 60 degrees C and 4 MPa, outperforming most reported results for BAD formation in a one-step process and even being comparable to those obtained by the two-step hydrogenation reaction route under much high temperatures and pressures. Crucially, we found that after facile alcohol (ethanol) treatment, an intriguing phenomenon of suppression of adjacent acid-assisted hydrogenolysis via extra acidic Al species at the NiO-Al2O3 interface is observed, contributing to the precise enhancement of BAD selectivity by inhibiting the production of butanol (BOL). This facile alcohol-treated method along with the revealed mechanism of blocked hydrogenolysis opens vast possibilities for designing high-performance and highly-selective hydrogenation catalysts. We have developed an efficient and robust alcohol-treated nickel-aluminum catalyst (NA-80E) applied to hydrogenate 2-butyne-1,4-diol (BYD) to butane-1,4-diol (BAD). The NA-80E catalyst achieved excellent BAD selectivity and yield (98.82 %) under mild reaction conditions. This was due to the removal of extra acidic Al species at the NiO-Al2O3 interface by alcohol treatment, which inhibited the side reaction and increased BAD selectivity.image
Keyword ：
alcohol-treated alcohol-treated BAD synthesis BAD synthesis nickel-based catalyst nickel-based catalyst selective hydrogenation selective hydrogenation
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| GB/T 7714 | Zhu, Caixia , He, Yingluo , Kushita, Ryotaro et al. Alcohol-Treated Nickel-Aluminium Catalyst for One-Step Highly-Selective Butane-1,4-Diol Synthesis from 2-Butyne-1,4-Diol [J]. | CHEMCATCHEM , 2023 , 16 (1) . |
| MLA | Zhu, Caixia et al. "Alcohol-Treated Nickel-Aluminium Catalyst for One-Step Highly-Selective Butane-1,4-Diol Synthesis from 2-Butyne-1,4-Diol" . | CHEMCATCHEM 16 . 1 (2023) . |
| APA | Zhu, Caixia , He, Yingluo , Kushita, Ryotaro , Peng, Xiaobo , Ma, Qingxiang , Liu, Guangbo et al. Alcohol-Treated Nickel-Aluminium Catalyst for One-Step Highly-Selective Butane-1,4-Diol Synthesis from 2-Butyne-1,4-Diol . | CHEMCATCHEM , 2023 , 16 (1) . |
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Cu-based bimetallic catalysts have been studied in the electrocatalytic nitrate (NO3-) reduction reaction (NO3-RR) for a long time. However, few studies have focused on horizontal comparison of CuNi, CuCo, and CuFe (abbreviated as CuM) bimetallic catalysts in electrocatalytic NO3-RR for ammonia synthesis. Herein, we prepare the three series of Cu-based bimetallic catalysts, with different atom ratios of Cu/M (Cu/M = 7/3, 5/5, or 3/7) and ordered mesoporous carbon (OMC) as support (denoted as CuM/OMC). The characterization results reveal that the metallic particles of Cu and M components possess an intimate relationship on the CuM/ OMC catalysts. The electrocatalytic NO3-RR performance uncovers that the optimal NH3 yield rates of CuM/ OMC catalysts at -0.8 V (vs reversible hydrogen electrode (RHE)) follow this order: Cu5Fe5/OMC > Cu5Co5/OMC > Cu7Ni3/OMC > Cu/OMC > Fe/OMC > Co/OMC > Ni/OMC > OMC. The bimetallic CuM/OMC catalysts exhibit higher NH3 yield rates than the monometallic catalysts. This is attributed to strong synergistic effects between the Cu and M components. We expect that these insights can stimulate new developments of bimetallic catalysts in electrocatalysis.
Keyword ：
Ammonia synthesis Ammonia synthesis Bimetal Bimetal Cu-based catalyst Cu-based catalyst Electrocatalytic nitrate reduction Electrocatalytic nitrate reduction Synergistic effect Synergistic effect
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| GB/T 7714 | Zhao, Jing , Liu, Lijuan , Yang, Ya et al. Insights into Electrocatalytic Nitrate Reduction to Ammonia via Cu-Based Bimetallic Catalysts [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2023 . |
| MLA | Zhao, Jing et al. "Insights into Electrocatalytic Nitrate Reduction to Ammonia via Cu-Based Bimetallic Catalysts" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING (2023) . |
| APA | Zhao, Jing , Liu, Lijuan , Yang, Ya , Liu, Dan , Peng, Xiaobo , Liang, Shijing et al. Insights into Electrocatalytic Nitrate Reduction to Ammonia via Cu-Based Bimetallic Catalysts . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2023 . |
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3D printing technology can rapidly transform digital model into physical realization, and has been widely studied in many fields. However, its developments are very slow in the fields of catalysis and reaction engineering, due to harsh application environments. Here, we report that metal 3D printing is used to prepare Nickel-based Self-Catalytic Reactor (Ni-SCR) for COx methanation. The optimized Ni-SCR samples exhibit unique surface properties. The catalytic results reveal that they also possess premium methanation performance. This work will facilitate the developments both in 3D printing technologies and novel catalytic systems.
Keyword ：
CO2 methanation CO2 methanation CO methanation CO methanation metal 3D printing metal 3D printing Nickel-based Self-Catalytic Reactor Nickel-based Self-Catalytic Reactor
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| GB/T 7714 | Wang, Chengwei , Peng, Xiaobo , He, Yingluo et al. Metal 3D Printed Nickel-Based Self-Catalytic Reactor for COx Methanation [J]. | CHEMCATCHEM , 2022 , 14 (12) . |
| MLA | Wang, Chengwei et al. "Metal 3D Printed Nickel-Based Self-Catalytic Reactor for COx Methanation" . | CHEMCATCHEM 14 . 12 (2022) . |
| APA | Wang, Chengwei , Peng, Xiaobo , He, Yingluo , Fan, Jiaqi , Lin, Xingyi , Jiang, Lilong et al. Metal 3D Printed Nickel-Based Self-Catalytic Reactor for COx Methanation . | CHEMCATCHEM , 2022 , 14 (12) . |
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Research on multifunctional catalysts for direct transformation of high-purity ethanol to butadiene has made some progress. However, the direct conversion of aqueous ethanol to butadiene (AETB) with high activity and butadiene selectivity, a very promising route for butadiene production, is still a considerable challenge. Here, we report a highly efficient multifunctional Y-ZnZr/Si-beta catalyst for the direct AETB conversion, and it exhibits an outstanding ethanol conversion of 80.2% and butadiene selectivity of 60.4%. The characterization results reveal that the rationally designed Y-ZnZr/Si-beta catalyst has synergy of each active sites and suitable balance of acid properties, which can promote the conversion of ethanol and the production of butadiene. Importantly, the experimental results prove that the rational coupling of various active sites plays a key role in significantly boosting the catalytic performance towards butadiene production. Moreover, the Y-ZnZr/Si-beta catalyst exhibits excellent regeneration ability. This work offers a promising catalytic design for direct AETB conversion.
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| GB/T 7714 | Wang, Kangzhou , Peng, Xiaobo , Wang, Chengwei et al. Selective direct conversion of aqueous ethanol into butadiene via rational design of multifunctional catalysts [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2022 , 12 (7) : 2210-2222 . |
| MLA | Wang, Kangzhou et al. "Selective direct conversion of aqueous ethanol into butadiene via rational design of multifunctional catalysts" . | CATALYSIS SCIENCE & TECHNOLOGY 12 . 7 (2022) : 2210-2222 . |
| APA | Wang, Kangzhou , Peng, Xiaobo , Wang, Chengwei , Gao, Weizhe , Liu, Na , Guo, Xiaoyu et al. Selective direct conversion of aqueous ethanol into butadiene via rational design of multifunctional catalysts . | CATALYSIS SCIENCE & TECHNOLOGY , 2022 , 12 (7) , 2210-2222 . |
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Ethanol, as one of the important bulk chemicals, is widely used in modern society. It can be produced by fermentation of sugar, petroleum refining, or conversion of syngas (CO/H-2). Among these approaches, conversion of syngas to ethanol (STE) is the most environmentally friendly and economical process. Although considerable progress has been made in STE conversion, control of CO activation and C-C growth remains a great challenge. This review highlights recent advances in the routes and catalysts employed in STE technology. The catalyst designs and pathway designs are summarized and analysed for the direct and indirect STE routes, respectively. In the direct STE routes (i.e., one-step synthesis of ethanol from syngas), modified catalysts of methanol synthesis, modified catalysts of Fischer-Tropsch synthesis, Mo-based catalysts, noble metal catalysts and multifunctional catalysts are systematically reviewed based on their catalyst designs. Further, in the indirect STE routes (i.e., multistep processes for ethanol synthesis from syngas via methanol/dimethyl ether as intermediates), carbonylation of methanol/dimethyl ether followed by hydrogenation, and coupling of methanol with CO to form dimethyl oxalate followed by hydrogenation, are outlined according to their pathway designs. The goal of this review is to provide a comprehensive perspective on STE technology and inspire the invention of new catalysts and pathway designs in the near future.
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| GB/T 7714 | Liu, Guangbo , Yang, Guohui , Peng, Xiaobo et al. Recent advances in the routes and catalysts for ethanol synthesis from syngas [J]. | CHEMICAL SOCIETY REVIEWS , 2022 , 51 (13) : 5606-5659 . |
| MLA | Liu, Guangbo et al. "Recent advances in the routes and catalysts for ethanol synthesis from syngas" . | CHEMICAL SOCIETY REVIEWS 51 . 13 (2022) : 5606-5659 . |
| APA | Liu, Guangbo , Yang, Guohui , Peng, Xiaobo , Wu, Jinhu , Tsubaki, Noritatsu . Recent advances in the routes and catalysts for ethanol synthesis from syngas . | CHEMICAL SOCIETY REVIEWS , 2022 , 51 (13) , 5606-5659 . |
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Reduction process is a key step to fabricate metal zeolite catalysts, but existing reduction technologies are always energy intensive and inevitably cause the agglomeration of metallic particles or destroy zeolite structure. Here the authors find that zeolites after ion exchange of ammonium display an interesting and unexpected self-reducing feature. Reduction process is a key step to fabricate metal-zeolite catalysts in catalytic synthesis. However, because of the strong interaction force, metal oxides in zeolites are very difficult to be reduced. Existing reduction technologies are always energy-intensive, and inevitably cause the agglomeration of metallic particles in metal-zeolite catalysts or destroy zeolite structure in severe cases. Herein, we disclose that zeolites after ion exchange of ammonium have an interesting and unexpected self-reducing feature. It can accurately control the reduction of metal-zeolite catalysts, via in situ ammonia production from 'ammonia pools', meanwhile, restrains the growth of the size of metals. Such new and reliable ammonia pool effect is not influenced by topological structures of zeolites, and works well on reducible metals. The ammonia pool effect is ultimately attributed to an atmosphere-confined self-regulation mechanism. This methodology will significantly promote the fabrication for metal-zeolite catalysts, and further facilitate design and development of low-cost and high-activity catalysts.
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| GB/T 7714 | Yao, Jie , He, Yingluo , Zeng, Yan et al. Ammonia pools in zeolites for direct fabrication of catalytic centers [J]. | NATURE COMMUNICATIONS , 2022 , 13 (1) . |
| MLA | Yao, Jie et al. "Ammonia pools in zeolites for direct fabrication of catalytic centers" . | NATURE COMMUNICATIONS 13 . 1 (2022) . |
| APA | Yao, Jie , He, Yingluo , Zeng, Yan , Feng, Xiaobo , Fan, Jiaqi , Komiyama, Shoya et al. Ammonia pools in zeolites for direct fabrication of catalytic centers . | NATURE COMMUNICATIONS , 2022 , 13 (1) . |
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