Pub Date : 2024-09-13DOI: 10.1007/s10562-024-04796-7
Qiong Wang, Kang Xiao, Haitao Li, Feng Lu, Quli Fan
A modified two-step coprecipitation method has been formulated to prepare a series of model CuZnO/Al2O3 catalysts for methanol synthesis from syngas. Evaluation at industrially relevant condition showed slightly higher activity and much higher stability for model catalysts than for a commercial catalyst. Due to the same CuZn-binary precursor, the model catalysts had similar structural properties with large specific surface area and pore volume, small CuO crystallites and good reducibility, resembling that of the commercial catalyst. However, the model catalysts showed much better uniformity of alumina distribution, which accounted for their better performance. Strong positive correlation between the deactivation rate and the coefficient of variation of Al/Zn indicates the uniformity of alumina distribution plays an important role in determining stability. Specifically, CuZnO/Al2O3 catalysts with alumina distributed more uniformly had higher stability. This work demonstrated that the formulated modified two-step coprecipitation could provide excellent CuZnO/Al2O3 catalysts for industrial applications. Additionally, it also affords new clues for the development of even better industrial catalysts.
{"title":"A Modified Two-Step Coprecipitation Method Provides Better CuZnO/Al2O3 Methanol Synthesis Catalyst with More Uniform Distribution of Alumina","authors":"Qiong Wang, Kang Xiao, Haitao Li, Feng Lu, Quli Fan","doi":"10.1007/s10562-024-04796-7","DOIUrl":"10.1007/s10562-024-04796-7","url":null,"abstract":"<div><p>A modified two-step coprecipitation method has been formulated to prepare a series of model CuZnO/Al<sub>2</sub>O<sub>3</sub> catalysts for methanol synthesis from syngas. Evaluation at industrially relevant condition showed slightly higher activity and much higher stability for model catalysts than for a commercial catalyst. Due to the same CuZn-binary precursor, the model catalysts had similar structural properties with large specific surface area and pore volume, small CuO crystallites and good reducibility, resembling that of the commercial catalyst. However, the model catalysts showed much better uniformity of alumina distribution, which accounted for their better performance. Strong positive correlation between the deactivation rate and the coefficient of variation of Al/Zn indicates the uniformity of alumina distribution plays an important role in determining stability. Specifically, CuZnO/Al<sub>2</sub>O<sub>3</sub> catalysts with alumina distributed more uniformly had higher stability. This work demonstrated that the formulated modified two-step coprecipitation could provide excellent CuZnO/Al<sub>2</sub>O<sub>3</sub> catalysts for industrial applications. Additionally, it also affords new clues for the development of even better industrial catalysts.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Different manganese salt precursor-doped g-C3N4 catalysts prepared by the mixed calcination method were applied in the heat-assisted visible light catalytic peroxymonosulfate (PMS) activation (Heat/Vis/PMS) system for the degradation of diclofenac (DCF). Under this Heat/Vis/PMS system, the CN-Mn-S catalyst using MnSO4 as the manganese salt precursor showed the optimal DCF degradation efficiency (96.9%) with the fastest reaction rate (0.1607 min−1). Besides, with the advantages of large specific surface area, high Mn3O4 generation, and good visible light absorption performance, CN-Mn-S catalyst also maintained excellent catalytic activity after five cycles. Electron paramagnetic resonance (EPR) analysis revealed that the generation of active species with relatively high contribution to DCF degradation, including generation of superoxide anion (O2·−) and singlet oxygen (1O2), were significantly increased in the CN-Mn-S/Heat/Vis/PMS system. Meanwhile, combined with the analysis of influence factor experiments and the DCF degradation characteristics, the CN-Mn-S/Heat/Vis/PMS system was able to maintain excellent DCF degradation ability in complex environments. This work provides a new idea for the application of PMS in real environment.
{"title":"Heat-Assisted Visible Light Catalytic PMS for Diclofenac Degradation: Mn-Doped g-C3N4 Catalysts and Synergistic Catalytic Mechanism","authors":"Qinglu Yuan, Peize Wang, Mengjie Fan, Yuan Xu, Yingwen Chen","doi":"10.1007/s10562-024-04817-5","DOIUrl":"10.1007/s10562-024-04817-5","url":null,"abstract":"<div><p>Different manganese salt precursor-doped g-C<sub>3</sub>N<sub>4</sub> catalysts prepared by the mixed calcination method were applied in the heat-assisted visible light catalytic peroxymonosulfate (PMS) activation (Heat/Vis/PMS) system for the degradation of diclofenac (DCF). Under this Heat/Vis/PMS system, the CN-Mn-S catalyst using MnSO<sub>4</sub> as the manganese salt precursor showed the optimal DCF degradation efficiency (96.9%) with the fastest reaction rate (0.1607 min<sup>−1</sup>). Besides, with the advantages of large specific surface area, high Mn<sub>3</sub>O<sub>4</sub> generation, and good visible light absorption performance, CN-Mn-S catalyst also maintained excellent catalytic activity after five cycles. Electron paramagnetic resonance (EPR) analysis revealed that the generation of active species with relatively high contribution to DCF degradation, including generation of superoxide anion (O<sub>2</sub>·<sup>−</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>), were significantly increased in the CN-Mn-S/Heat/Vis/PMS system. Meanwhile, combined with the analysis of influence factor experiments and the DCF degradation characteristics, the CN-Mn-S/Heat/Vis/PMS system was able to maintain excellent DCF degradation ability in complex environments. This work provides a new idea for the application of PMS in real environment.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254155","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-13DOI: 10.1007/s10562-024-04813-9
Jingru Hu, Minjun Jiang, Bingwen Hu, Gang Cheng
Remediation of antibiotics by photocatalysis technique has been regarded as a promising route to tackle with the environmental pollution affecting human survival and development. In this work, brookite TiO2 nanorods with different oxygen vacancy have been synthesized through tailoring the volume of ethylene glycol by hydrothermally treatment with NaTiOx-nanoassembly. After constitute and morphology confirmation with different characterizations, their photocatalytic performances are evaluated via ciprofloxacin (CIP) antibiotic degradation experiments. The result shows that the TiO2-0 has the highest photocatalytic efficiency towards CIP degradation, comparing with TiO2-15 and TiO2-30 samples. Although the TiO2-30 has high concentration oxygen vacancy, it exhibits excellent adsorption ability in the dark, rather than CIP degradation rate. The photo/electrochemical tests suggest the photo-generated electron lifetime, charge transfer ability, and the effective active sites on the material’s surface are inversely proportional to the concentration of oxygen vacancies. It also concludes that rational fabrication conditions tailoring of the photocatalyst could optimize the corresponding capability in the antibiotic degradation process. In addition, the possible degradation pathway is also proposed based on the high resolution mass spectrometry (HRMS), and the acute toxicity changes in the degradation process are also predicted.
{"title":"Fabrication Condition-Dependent Photocatalytic Ciprofloxacin (CIP) Antibiotic Degradation of NaTiOx-Derived Brookite TiO2 Nanorods","authors":"Jingru Hu, Minjun Jiang, Bingwen Hu, Gang Cheng","doi":"10.1007/s10562-024-04813-9","DOIUrl":"10.1007/s10562-024-04813-9","url":null,"abstract":"<div><p>Remediation of antibiotics by photocatalysis technique has been regarded as a promising route to tackle with the environmental pollution affecting human survival and development. In this work, brookite TiO<sub>2</sub> nanorods with different oxygen vacancy have been synthesized through tailoring the volume of ethylene glycol by hydrothermally treatment with NaTiOx-nanoassembly. After constitute and morphology confirmation with different characterizations, their photocatalytic performances are evaluated via ciprofloxacin (CIP) antibiotic degradation experiments. The result shows that the TiO<sub>2</sub>-0 has the highest photocatalytic efficiency towards CIP degradation, comparing with TiO<sub>2</sub>-15 and TiO<sub>2</sub>-30 samples. Although the TiO<sub>2</sub>-30 has high concentration oxygen vacancy, it exhibits excellent adsorption ability in the dark, rather than CIP degradation rate. The photo/electrochemical tests suggest the photo-generated electron lifetime, charge transfer ability, and the effective active sites on the material’s surface are inversely proportional to the concentration of oxygen vacancies. It also concludes that rational fabrication conditions tailoring of the photocatalyst could optimize the corresponding capability in the antibiotic degradation process. In addition, the possible degradation pathway is also proposed based on the high resolution mass spectrometry (HRMS), and the acute toxicity changes in the degradation process are also predicted.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175705","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-12DOI: 10.1007/s10562-024-04807-7
Samah Zaki Naji, Ching Thian Tye, Abdul Rahman Mohamed
The increasing global demand for fuel, along with pressing environmental regulations and concerns, and the need for energy security, all point to the biofuel industry seeing rapid growth in the near future. The objective of this study was to study the performance of a series of activated carbon (AC) supported La and Ce oxide catalysts in the catalytic cracking of waste cooking oil into alkane-based hydrocarbon. Coconut-shell activated carbon was loaded with various amounts of lanthanum and cerium were prepared via wet impregnation. The catalytic cracking activity was evaluated in a fixed bed reactor under N2 flow at 450 °C and a weight hourly space velocity of 8 h−1 at 60 min. The physical and chemical properties of the prepared catalysts were characterized by BET, SEM–EDX, XRD, TPD-NH3/CO2, FTIR, and TGA. The results indicated that 5 wt% La/AC performed superiorly with a liquid product of 87.03% which composed of 99.09% hydrocarbons, that were mostly alkane (79.89%) with n-(C15 + C17) 66% selectivity (66.13%).
{"title":"Catalytic Cracking of Waste Cooking Oil to Alkane-Based Hydrocarbon Over Activated Carbon Supported La and Ce Oxides","authors":"Samah Zaki Naji, Ching Thian Tye, Abdul Rahman Mohamed","doi":"10.1007/s10562-024-04807-7","DOIUrl":"10.1007/s10562-024-04807-7","url":null,"abstract":"<div><p>The increasing global demand for fuel, along with pressing environmental regulations and concerns, and the need for energy security, all point to the biofuel industry seeing rapid growth in the near future. The objective of this study was to study the performance of a series of activated carbon (AC) supported La and Ce oxide catalysts in the catalytic cracking of waste cooking oil into alkane-based hydrocarbon. Coconut-shell activated carbon was loaded with various amounts of lanthanum and cerium were prepared via wet impregnation. The catalytic cracking activity was evaluated in a fixed bed reactor under N<sub>2</sub> flow at 450 °C and a weight hourly space velocity of 8 h<sup>−1</sup> at 60 min. The physical and chemical properties of the prepared catalysts were characterized by BET, SEM–EDX, XRD, TPD-NH<sub>3</sub>/CO<sub>2</sub>, FTIR, and TGA. The results indicated that 5 wt% La/AC performed superiorly with a liquid product of 87.03% which composed of 99.09% hydrocarbons, that were mostly alkane (79.89%) with n-(C<sub>15</sub> + C<sub>17</sub>) 66% selectivity (66.13%).</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Copper-Nitrogen-Carbon (Cu-N-C) materials, derived from zeolite imidazolium frameworks, serve as promising carriers for catalyzing glycerol carbonylation reactions due to their modifiable pore size structure, enhanced catalytic selectivity, and stability. However, conventional palladium loading often results in the susceptibility of Cu-Pd co-catalysis loss, impeding practical application. In this investigation, we employed an in-situ confinement technique to embed polyvinylpyrrolidone (PVP)-modified palladium nanoparticles within the Cu-ZIF-8 metal framework, followed by direct calcination under a nitrogen atmosphere. This method yielded uniform-sized and shaped copper-palladium alloy catalysts, denoted as Pd@Cu-NC. Comparative analysis with catalysts prepared via impregnation followed by calcination revealed significantly enhanced stability of the resulting Pd@Cu-NC catalysts, with improved selectivity and stability of the active components. Notably, catalyst stability was markedly improved, and active component loss was mitigated. Under optimized conditions, a remarkable yield of 90.14% and selectivity of 99.91% were achieved, while retaining 77.43% activity after five cycles. Furthermore, density functional theory (DFT) calculations were employed to simulate the kinetics of carbon monoxide adsorption and glycerol dimethyl acetal (DMA) solution on various substrates. The presence of copper oxide notably reduced the adsorption energy of substrates to carbon monoxide and reaction solutions, thereby lowering the reaction activation energy and enhancing the reaction rate. This computational analysis provides further evidence of the beneficial role of copper oxide in facilitating the carbonylation reaction.
{"title":"Confinement of Ultrasmall Pd Clusters Within Nanosized ZIF-8-Derived Cu-N-C Materials for Efficient and Stable Synthesis of Glycerol Carbonate from Glycerol","authors":"Jiawen Zhang, Zhihao Lv, Pingbo Zhang, Mingming Fan, Pingping Jiang, Yan Leng","doi":"10.1007/s10562-024-04799-4","DOIUrl":"10.1007/s10562-024-04799-4","url":null,"abstract":"<div><p>Copper-Nitrogen-Carbon (Cu-N-C) materials, derived from zeolite imidazolium frameworks, serve as promising carriers for catalyzing glycerol carbonylation reactions due to their modifiable pore size structure, enhanced catalytic selectivity, and stability. However, conventional palladium loading often results in the susceptibility of Cu-Pd co-catalysis loss, impeding practical application. In this investigation, we employed an in-situ confinement technique to embed polyvinylpyrrolidone (PVP)-modified palladium nanoparticles within the Cu-ZIF-8 metal framework, followed by direct calcination under a nitrogen atmosphere. This method yielded uniform-sized and shaped copper-palladium alloy catalysts, denoted as Pd@Cu-NC. Comparative analysis with catalysts prepared via impregnation followed by calcination revealed significantly enhanced stability of the resulting Pd@Cu-NC catalysts, with improved selectivity and stability of the active components. Notably, catalyst stability was markedly improved, and active component loss was mitigated. Under optimized conditions, a remarkable yield of 90.14% and selectivity of 99.91% were achieved, while retaining 77.43% activity after five cycles. Furthermore, density functional theory (DFT) calculations were employed to simulate the kinetics of carbon monoxide adsorption and glycerol dimethyl acetal (DMA) solution on various substrates. The presence of copper oxide notably reduced the adsorption energy of substrates to carbon monoxide and reaction solutions, thereby lowering the reaction activation energy and enhancing the reaction rate. This computational analysis provides further evidence of the beneficial role of copper oxide in facilitating the carbonylation reaction.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-12DOI: 10.1007/s10562-024-04806-8
Dalei Sun, Kang Cheng, Chen Zhou, Xiangye Liu, Zhiwu Liang
CO2 regeneration and reutilization is considered to be a green and effective route with highly potential for development. CeO2 showed high catalytic activity for the production of N,N′-dibutylurea through n-butyl amine and CO2. Herein, V-doped CeO2 with different molar ratios of V/Ce (Vx%-CeO2, x = 0, 0.4, 0.6, 0.8 and 1.0) were further successfully synthesized and firstly applied to the reaction of CO2 with n-butyl amine. The reaction results displayed the catalytic performance of CeO2 were prominently enhanced by doping V5+ and followed an order of V0.8%-CeO2 > V0.6%-CeO2 > V1.0%-CeO2 > V0.4%-CeO2 > CeO2. The reason for the changes in the catalytic activities of CeO2 with different doping amounts of V5+ could be closely related to the surface oxygen vacancy and surface weak acidity and weak basicity based on specific analysis of relevant characterization including XRD, BET, Raman, XPS, EPR and NH3/CO2-TPD.
{"title":"Enhanced the Catalytic Performance of CeO2 by Tuning V5+ Doping Amount in Carbonylation of n-Butyl Amine with CO2","authors":"Dalei Sun, Kang Cheng, Chen Zhou, Xiangye Liu, Zhiwu Liang","doi":"10.1007/s10562-024-04806-8","DOIUrl":"10.1007/s10562-024-04806-8","url":null,"abstract":"<div><p>CO<sub>2</sub> regeneration and reutilization is considered to be a green and effective route with highly potential for development. CeO<sub>2</sub> showed high catalytic activity for the production of N,N′-dibutylurea through n-butyl amine and CO<sub>2</sub>. Herein, V-doped CeO<sub>2</sub> with different molar ratios of V/Ce (V<sub>x%</sub><i>-</i>CeO<sub>2</sub>, x = 0, 0.4, 0.6, 0.8 and 1.0) were further successfully synthesized and firstly applied to the reaction of CO<sub>2</sub> with n-butyl amine. The reaction results displayed the catalytic performance of CeO<sub>2</sub> were prominently enhanced by doping V<sup>5+</sup> and followed an order of V<sub>0.8%</sub>-CeO<sub>2</sub> > V<sub>0.6%</sub>-CeO<sub>2</sub> > V<sub>1.0%</sub>-CeO<sub>2</sub> > V<sub>0.4%</sub>-CeO<sub>2</sub> > CeO<sub>2</sub>. The reason for the changes in the catalytic activities of CeO<sub>2</sub> with different doping amounts of V<sup>5+</sup> could be closely related to the surface oxygen vacancy and surface weak acidity and weak basicity based on specific analysis of relevant characterization including XRD, BET, Raman, XPS, EPR and NH<sub>3</sub>/CO<sub>2</sub>-TPD.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175694","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-11DOI: 10.1007/s10562-024-04809-5
Long Tang, Xingyun Liu, Zeyong Zhu, Junjie Luo, Song Zhao, Wenyi Wang
The Co/Co-Nx-embedded mesoporous 3D flower-like carbon sheet (Co/Co-N-MC-800) catalyst is successfully prepared from high N content H-1,2,4-Triazol-3-amine organic-ligand at different pyrolysis temperatures based on in situ pyrolysis Co-metal organic frame (MOF) (Co-PTA-MOF) precursor under nitrogen. The metal active center of the mesoporous Co/Co-N-MC-800 catalyst with more defect sites is situated in the positively charged 0 ~ + 2, and the bond spacing is consistent with the Co-N4 plane structure of the co-porphyrin. The obtained Co/Co-N-MC-800 possesses an excellent oxygen reduction reaction performance with a higher onset potential (0.92 V vs RHE) and half-wave potential (0.76 V vs RHE), which is closer to Pt/C and outstanding long-term stability with 89.1% current retention after 89 h and displays an optional power density of 1079.3 ± 22.5mW·m−2 in air-breath cathode microbial fuel cell (MFC). The improved catalytic performance maybe attributes to combination of the special 3D nanostructure, embedded cobalt nanoparticles (forming Co-Nx) and N-doped mesoporous carbon sheet material. The present study provides the technical and theoretical basis for the ORR through the cathode modification of MOF prepared from non-precious metal and N content organic-ligand.
Graphical Abstract
以氮气条件下原位热解钴-金属有机框架（MOF）（Co-PTA-MOF）前驱体为基础，在不同热解温度下以高N含量的H-1,2,4-三唑-3-胺有机配体为原料，成功制备了Co/Co-Nx嵌入介孔三维花状碳片（Co/Co-N-MC-800）催化剂。缺陷位点较多的介孔 Co/Co-N-MC-800 催化剂的金属活性中心位于带正电的 0 ~ + 2 处，键间距与共卟啉的 Co-N4 平面结构一致。所获得的 Co/Co-N-MC-800 具有优异的氧还原反应性能，其起始电位（0.92 V vs RHE）和半波电位（0.76 V vs RHE）更接近于 Pt/C，并且具有出色的长期稳定性，89 h 后的电流保持率为 89.1%，在空气呼吸阴极微生物燃料电池（MFC）中的可选功率密度为 1079.3 ± 22.5mW-m-2。催化性能的提高可能归功于特殊的三维纳米结构、嵌入式钴纳米颗粒（形成 Co-Nx）和掺杂 N 的介孔碳片材料的结合。本研究为利用非贵金属和含 N 有机配体制备的 MOF 阴极改性实现 ORR 提供了技术和理论依据。
{"title":"Metal Organic Framework–Derived Co and Co-Nx Embedded Mesoporous Carbon Sheets as an Efficient Electrocatalyst Toward the Oxygen Reduction Reaction for Air-Breath Cathode Microbial Fuel Cells","authors":"Long Tang, Xingyun Liu, Zeyong Zhu, Junjie Luo, Song Zhao, Wenyi Wang","doi":"10.1007/s10562-024-04809-5","DOIUrl":"10.1007/s10562-024-04809-5","url":null,"abstract":"<div><p>The Co/Co-N<i>x</i>-embedded mesoporous 3D flower-like carbon sheet (Co/Co-N-MC-800) catalyst is successfully prepared from high N content H-1,2,4-Triazol-3-amine organic-ligand at different pyrolysis temperatures based on in situ pyrolysis Co-metal organic frame (MOF) (Co-PTA-MOF) precursor under nitrogen. The metal active center of the mesoporous Co/Co-N-MC-800 catalyst with more defect sites is situated in the positively charged 0 ~ + 2, and the bond spacing is consistent with the Co-N<sub>4</sub> plane structure of the co-porphyrin. The obtained Co/Co-N-MC-800 possesses an excellent oxygen reduction reaction performance with a higher onset potential (0.92 V <i>vs</i> RHE) and half-wave potential (0.76 V <i>vs</i> RHE), which is closer to Pt/C and outstanding long-term stability with 89.1% current retention after 89 h and displays an optional power density of 1079.3 ± 22.5mW·m<sup>−2</sup> in air-breath cathode microbial fuel cell (MFC). The improved catalytic performance maybe attributes to combination of the special 3D nanostructure, embedded cobalt nanoparticles (forming Co-N<sub><i>x</i></sub>) and N-doped mesoporous carbon sheet material. The present study provides the technical and theoretical basis for the ORR through the cathode modification of MOF prepared from non-precious metal and N content organic-ligand.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-11DOI: 10.1007/s10562-024-04798-5
Mei Ma, Zhihua Liu, Jianguo Zhou
The decomposition mechanism of dyes under the synergistic effect of pyroelectric catalysis and photocatalysis was systematically investigated using a BaTiO3/NiB catalyst in this paper, and the degradation efficiency of BaTiO3/NiB was 97.5% under light and 24 cycles of hot and cold at 25 ~ 65 °C, showing high pyroelectroic catalytic RhB decomposition activity and excellent recoverability. The degradation rate constants of RhB chromophore degradation by Pyro-photocatalytic coupled were 3.2 times as high as those of photocatalysis and 11.8 times as high as those of pyroelectric catalysis. In this study, we used light-assisted electrodeposition to deposit a thin layer of amorphous NiB acid salts onto the surface of a BaTiO3 photoelectrode aiming to explore its influence on photocharge separation and the catalytic mechanism of NiB in the context of pollutant degradation. The synergies between the pyroelectric internal field and the amorphous Ni–B acid salt thin layer during photogenerated charge separation were extensively explored in this paper, including the introduction of a port for pyroelectric polarization.
{"title":"Enhanced Pyro-Photo Catalysis of the BaTiO3/NiB Catalyst for Dye Degradation Driven by Visible Light and Cold–Hot Cycles","authors":"Mei Ma, Zhihua Liu, Jianguo Zhou","doi":"10.1007/s10562-024-04798-5","DOIUrl":"10.1007/s10562-024-04798-5","url":null,"abstract":"<div><p>The decomposition mechanism of dyes under the synergistic effect of pyroelectric catalysis and photocatalysis was systematically investigated using a BaTiO<sub>3</sub>/NiB catalyst in this paper, and the degradation efficiency of BaTiO<sub>3</sub>/NiB was 97.5% under light and 24 cycles of hot and cold at 25 ~ 65 °C, showing high pyroelectroic catalytic RhB decomposition activity and excellent recoverability. The degradation rate constants of RhB chromophore degradation by Pyro-photocatalytic coupled were 3.2 times as high as those of photocatalysis and 11.8 times as high as those of pyroelectric catalysis. In this study, we used light-assisted electrodeposition to deposit a thin layer of amorphous NiB acid salts onto the surface of a BaTiO<sub>3</sub> photoelectrode aiming to explore its influence on photocharge separation and the catalytic mechanism of NiB in the context of pollutant degradation. The synergies between the pyroelectric internal field and the amorphous Ni–B acid salt thin layer during photogenerated charge separation were extensively explored in this paper, including the introduction of a port for pyroelectric polarization.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-11DOI: 10.1007/s10562-024-04827-3
Kefeng Shang, Xi Feng, Yongxin Wang
MgCoFe layered double oxides (MgCoFe-LDO) were fabricated to activate peroxymonosulfate (PMS) for degradation of sulfamethoxazole (SMX), and the highly efficient degradation of SMX revealed an excellent catalytic activity of Mg2Co1Fe1-LDO for PMS under different pH values and water matrix. Scanning electron microscope analysis indicated the catalyst has a typical “flower-like” structure, and the X-ray powder diffraction analyses proved that the main crystal phase of Mg2Co1Fe1-LDO is CoFe2O4 and Mg1−xFexO, which is responsible for the good catalytic activity of Mg2Co1Fe1-LDO. The radical scavenging experiments confirmed that 1O2, ({text{SO}}_{4}^{cdot - }), OH and ({text{O}}_{2}^{cdot - }) were involved in the degradation of SMX, but 1O2 and ({text{SO}}_{4}^{cdot - }) played the dominant roles. According to the X-ray photoelectron spectroscopy (XPS) of Mg2Co1Fe1-LDO catalyst, it was referred that the species including CoOH+, CoO+, Fe3+, FeOH2+, Fe2+, etc. involve in the activation process of PMS. Moreover, the possible degradation pathways of SMX were proposed according to the detected intermediates including N-hydroxy sulfamethoxazole, 3-amino-5-methylisoxazole from LC–MS analysis, and the toxicity analysis via Toxicity Estimation Software Tool software shows that most of the degradation products of SMX have lower toxicity than SMX.
{"title":"Efficient Degradation of Sulfamethoxazole via Reactive Oxygen Species Produced from Activated Peroxymonosulfate by MgCoFe-LDO Catalyst","authors":"Kefeng Shang, Xi Feng, Yongxin Wang","doi":"10.1007/s10562-024-04827-3","DOIUrl":"10.1007/s10562-024-04827-3","url":null,"abstract":"<div><p>MgCoFe layered double oxides (MgCoFe-LDO) were fabricated to activate peroxymonosulfate (PMS) for degradation of sulfamethoxazole (SMX), and the highly efficient degradation of SMX revealed an excellent catalytic activity of Mg<sub>2</sub>Co<sub>1</sub>Fe<sub>1</sub>-LDO for PMS under different pH values and water matrix. Scanning electron microscope analysis indicated the catalyst has a typical “flower-like” structure, and the X-ray powder diffraction analyses proved that the main crystal phase of Mg<sub>2</sub>Co<sub>1</sub>Fe<sub>1</sub>-LDO is CoFe<sub>2</sub>O<sub>4</sub> and Mg<sub>1−x</sub>Fe<sub>x</sub>O, which is responsible for the good catalytic activity of Mg<sub>2</sub>Co<sub>1</sub>Fe<sub>1</sub>-LDO. The radical scavenging experiments confirmed that <sup>1</sup>O<sub>2</sub>, <span>({text{SO}}_{4}^{cdot - })</span>, OH and <span>({text{O}}_{2}^{cdot - })</span> were involved in the degradation of SMX, but <sup>1</sup>O<sub>2</sub> and <span>({text{SO}}_{4}^{cdot - })</span> played the dominant roles. According to the X-ray photoelectron spectroscopy (XPS) of Mg<sub>2</sub>Co<sub>1</sub>Fe<sub>1</sub>-LDO catalyst, it was referred that the species including CoOH<sup>+</sup>, CoO<sup>+</sup>, Fe<sup>3+</sup>, FeOH<sup>2+</sup>, Fe<sup>2+</sup>, etc. involve in the activation process of PMS. Moreover, the possible degradation pathways of SMX were proposed according to the detected intermediates including N-hydroxy sulfamethoxazole, 3-amino-5-methylisoxazole from LC–MS analysis, and the toxicity analysis via Toxicity Estimation Software Tool software shows that most of the degradation products of SMX have lower toxicity than SMX.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175712","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-11DOI: 10.1007/s10562-024-04816-6
Yijin Qin, Yan Li, Liang Wei, Meng Li, Hongxi Zhang, Jing Yang, Xiande Yang
The heterojunction construction through the effective combination of two metal sulfides can significantly improve the photocatalytic performance in the visible light region. In order to improve the photocatalytic efficiency of molybdenum disulfide (MoS2), we synthesized a series of CdS/MoS2 (CM) composites using a simple hydrothermal method. Their photocatalytic activities were evaluated by the photocatalytic hydrogen production. The results showed that the photocatalytic hydrogen production rate of CM composites was significantly enhanced after visible light irradiation, which was attributed to the improvement of visible light absorption capacity, efficient separation of photogenerated carriers, strong photocurrent response, and fast charge mobility. What’s more, sample CM-3 exhibited the highest photocatalytic hydrogen production efficiency of 2809.4 μmol g−1 h−1 compared to pure MoS2 (0 μmol g−1 h−1) and CdS (81.5 μmol g−1 h−1). Therefore, the successful construction of heterojunction can accumulate much more photogenerated electrons for MoS2, which is favorable to enhance its photocatalytic hydrogen production. This study provides strong evidence that heterojunction construction can obviously improve the photocatalytic activity.
Graphical Abstract
Photocatalytic H2 production of CM-3 composite. MoS2 constructed heterojunction with CdS can effectively improve the photocatalytic activity. The photocatalytic H2 production rate of CdS/MoS2 composite can reach 2809.4 μmol g-1 h-1
{"title":"Electron Density Optimization of Molybdenum Disulfide for Enhanced Photocatalytic Hydrogen Production Performance","authors":"Yijin Qin, Yan Li, Liang Wei, Meng Li, Hongxi Zhang, Jing Yang, Xiande Yang","doi":"10.1007/s10562-024-04816-6","DOIUrl":"10.1007/s10562-024-04816-6","url":null,"abstract":"<div><p>The heterojunction construction through the effective combination of two metal sulfides can significantly improve the photocatalytic performance in the visible light region. In order to improve the photocatalytic efficiency of molybdenum disulfide (MoS<sub>2</sub>), we synthesized a series of CdS/MoS<sub>2</sub> (CM) composites using a simple hydrothermal method. Their photocatalytic activities were evaluated by the photocatalytic hydrogen production. The results showed that the photocatalytic hydrogen production rate of CM composites was significantly enhanced after visible light irradiation, which was attributed to the improvement of visible light absorption capacity, efficient separation of photogenerated carriers, strong photocurrent response, and fast charge mobility. What’s more, sample CM-3 exhibited the highest photocatalytic hydrogen production efficiency of 2809.4 μmol g<sup>−1</sup> h<sup>−1</sup> compared to pure MoS<sub>2</sub> (0 μmol g<sup>−1</sup> h<sup>−1</sup>) and CdS (81.5 μmol g<sup>−1</sup> h<sup>−1</sup>). Therefore, the successful construction of heterojunction can accumulate much more photogenerated electrons for MoS<sub>2</sub>, which is favorable to enhance its photocatalytic hydrogen production. This study provides strong evidence that heterojunction construction can obviously improve the photocatalytic activity.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div><div><p>Photocatalytic H2 production of CM-3 composite. MoS2 constructed heterojunction with CdS can effectively improve the photocatalytic activity. The photocatalytic H2 production rate of CdS/MoS2 composite can reach 2809.4 μmol g-1 h-1</p></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175713","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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