Applied Catalysis B: Environmental最新文献

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CO2 to dimethylcarbonate synthesis: surface defects and oxygen vacancies engineering on MOF-derived CexZr1-xO2-y catalysts 二氧化碳到碳酸二甲酯的合成:源自 MOF 的 CexZr1-xO2-y 催化剂上的表面缺陷和氧空位工程
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-15 DOI: 10.1016/j.apcatb.2024.123723
Sergio Rojas-Buzo, Davide Salusso, Andrea Jouve, Edoardo Bracciotti, Matteo Signorile, Silvia Bordiga
{"title":"CO2 to dimethylcarbonate synthesis: surface defects and oxygen vacancies engineering on MOF-derived CexZr1-xO2-y catalysts","authors":"Sergio Rojas-Buzo, Davide Salusso, Andrea Jouve, Edoardo Bracciotti, Matteo Signorile, Silvia Bordiga","doi":"10.1016/j.apcatb.2024.123723","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.123723","url":null,"abstract":"<p>Direct reaction of carbon dioxide and methanol to produce dimethylcarbonate (DMC) is an interesting process that allows the synthesis of such valuable product in a more environmentally friendly route than the present technology that is expensive, unsafe and use toxic raw materials. Unfortunately, this alternative presents intrinsic limitations as the low yield due to thermodynamic limitation and reaction mechanism remains unclear. Herein, we propose a reproducible synthetic methodology of cerium oxide and Ce/Zr oxide solid solutions by calcination of opportune UiO-66(Ce/Zr) MOFs, employed as sacrificial precursors. The higher defectivity of these nanomaterials, corroborated by IR of adsorbed CO, in comparison with commercially-available ones, as those synthesized by traditional sol-gel methods, plays a pivotal role in the direct synthesis of DMC. Lastly, reaction mechanism was systematically and in-depth investigated by <em>in situ</em> AP-NEXAFS and MCR-ALS/LCF augmented IR spectroscopy, unveiling the role of oxygen vacancies towards CH<sub>3</sub>OH activation.</p>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139469256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Single-atom Pt–N4 active sites anchored on porous C3N4 nanosheet for boosting the photocatalytic CO2 reduction with nearly 100% CO selectivity 在多孔 C3N4 纳米片上锚定单原子 Pt-N4 活性位点,以接近 100% 的 CO 选择性提高光催化 CO2 还原效率
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-15 DOI: 10.1016/j.apcatb.2024.123737
Shan Hu , Panzhe Qiao , Xinming Liang , Guiming Ba , Xiaolong Zu , Huilin Hu , Jinhua Ye , Defa Wang
{"title":"Single-atom Pt–N4 active sites anchored on porous C3N4 nanosheet for boosting the photocatalytic CO2 reduction with nearly 100% CO selectivity","authors":"Shan Hu ,&nbsp;Panzhe Qiao ,&nbsp;Xinming Liang ,&nbsp;Guiming Ba ,&nbsp;Xiaolong Zu ,&nbsp;Huilin Hu ,&nbsp;Jinhua Ye ,&nbsp;Defa Wang","doi":"10.1016/j.apcatb.2024.123737","DOIUrl":"10.1016/j.apcatb.2024.123737","url":null,"abstract":"<div><p>Photoreduction of CO<sub>2</sub> and H<sub>2</sub>O into fuels and value-added chemicals is a promising green technology for solar-to-chemical conversion. However, improving the conversion efficiency with regulated product selectivity is a big challenge due to the sluggish dynamic transfer and insufficient active sites. Herein, we report on Pt single atoms anchored porous C<sub>3</sub>N<sub>4</sub><span> nanosheet photocatalyst (Pt</span><sub>1</sub>@CN) with Pt–N<sub>4</sub> coordination for stable and efficient CO<sub>2</sub> photoreduction using H<sub>2</sub>O as reductant. The Pt<sub>1</sub>@CN exhibits an evolution rate of 84.8 μmol g<sup>−1</sup> h<sup>−1</sup> with nearly 100% CO selectivity, outperforming most previous C<sub>3</sub>N<sub>4</sub>-based single-atom photocatalysts. Experimental and DFT calculation results reveal that the Pt–N<sub>4</sub> coordinated active sites promote the photogenerated electron transfer, CO<sub>2</sub> adsorption/activation, *COOH generation, and *CO desorption, thus accounting for the significantly improved CO<sub>2</sub> photoreduction activity with ∼100% CO selectivity. This study provides a deep insight into the significant roles of single-atom active sites in enhancing the CO<sub>2</sub> photoreduction activity and regulating the product selectivity.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139475469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanisms and Site Requirements for NO and NH3 oxidation on Cu/SSZ-13 Cu/SSZ-13 上氧化 NO 和 NH3 的机理和场地要求
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-15 DOI: 10.1016/j.apcatb.2024.123726
Yilin Wang, Runze Zhao, Kenneth G. Rappé, Yong Wang, Fanglin Che, Feng Gao
{"title":"Mechanisms and Site Requirements for NO and NH3 oxidation on Cu/SSZ-13","authors":"Yilin Wang, Runze Zhao, Kenneth G. Rappé, Yong Wang, Fanglin Che, Feng Gao","doi":"10.1016/j.apcatb.2024.123726","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.123726","url":null,"abstract":"<p>Two series of Cu/SSZ-13 catalysts were synthesized via aqueous solution and solid-state ion exchange using SSZ-13 supports of varying Si/Al ratios. The isolated and multinuclear Cu content of these catalysts were determined by H<sub>2</sub> temperature programmed reduction (H<sub>2</sub>-TPR). Multinuclear Cu in these catalysts, including in situ Cu-dimers formed from ZCu<sup>II</sup>OH coupling and permanent CuO clusters, are active species for dry NO oxidation. NH<sub>3</sub> oxidation on these catalysts follows an internal SCR (i-SCR) mechanism, i.e., a portion of NH<sub>3</sub> is first oxidized to NO, then NO is selectively reduced by the remaining NH<sub>3</sub> to N<sub>2</sub>. NH<sub>3</sub> oxidation displays distinct kinetic behavior below ~300 °C and above ~400 °C. At low temperature the results indicate that NH<sub>3</sub>-solvated mobile Cu-ions are the active centers. CuO clusters, when present, also contribute to the low temperature activity by catalyzing NH<sub>3</sub> oxidation to NO. At high temperature, in situ Cu-dimers and CuO clusters catalyze NH<sub>3</sub> oxidation to NO, and isolated Cu-ions catalyze SCR to realize the cascade turnovers. For both NO and NH<sub>3</sub> oxidation, Cu-dimers balanced by framework charges of close proximity appear to be more active than Cu-dimers balanced by distant framework charges. However, the former Cu-dimers are less stable than the latter and tend to split into monomers in the presence of vicinal Brønsted acid sites. Via density functional theory (DFT) calculations, the i-SCR mechanism for low temperature NH<sub>3</sub> oxidation, i.e., the energetic favorability for the involvement of the NO intermediate, is justified. The DFT results also agree with experimental data that the formation of Cu-dimers from ZCu<sup>II</sup>OH dimerization is essential for NH<sub>3</sub> oxidation at high temperature.</p>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139468962","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ligand Bridged MXene/Metal Organic Frameworks Heterojunction for Efficient Photocatalytic Ammonia Synthesis 配体桥接 MXene/金属有机框架异质结用于高效光催化氨合成
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-15 DOI: 10.1016/j.apcatb.2024.123732
Zhengfeng Shen, Feifei Li, Lijun Guo, Xiaochao Zhang, Yawen Wang, Yunfang Wang, Xuan Jian, Xiaoming Gao, Zhongde Wang, Rui Li, Caimei Fan, Jianxin Liu
{"title":"Ligand Bridged MXene/Metal Organic Frameworks Heterojunction for Efficient Photocatalytic Ammonia Synthesis","authors":"Zhengfeng Shen, Feifei Li, Lijun Guo, Xiaochao Zhang, Yawen Wang, Yunfang Wang, Xuan Jian, Xiaoming Gao, Zhongde Wang, Rui Li, Caimei Fan, Jianxin Liu","doi":"10.1016/j.apcatb.2024.123732","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.123732","url":null,"abstract":"<p>Efficient interfacial charge transfer is imperative for enhancing N<sub>2</sub> photofixation, yet controlling this process proves challenging. Herein, a unique ligand pre-coupling strategy was employed to design ligand-bridged MXene/MIL-125(Ti), creating a coordination bond between Ti<sub>3</sub>C<sub>2</sub>O<sub>x</sub> and MIL125(Ti) and forming a ligand-bridge, aiming to regulate interfacial electron transfer. Kelvin probe force microscopy and charge density difference analysis revealed the establishment of an electronic unidirectional transport channel from MIL-125(Ti) to Ti<sub>3</sub>C<sub>2</sub>O<sub>x</sub> through this ligand-bridge. This effectively reduced the interface charge transfer resistance, enhanced the separation efficiency of charge carriers. Consequently, the Ti<sub>3</sub>C<sub>2</sub>O<sub>x</sub>/MIL-125(Ti) manifested an excellent ammonia evolution rate of 103.02 μmol·g<sub>cat</sub><sup>-1</sup>·h<sup>-1</sup>. Furthermore, the efficiency of this strategy for accelerating the separation of photogenerated carriers was demonstrated in five other MOFs, demonstrating its potential for constructing ligand-bridged MXene/MOFs heterojunctions.</p>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139475688","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Extraordinary d–d hybridization in Co(Cu)0.5OxHy microcubes facilitates PhCH2O* –Co(Ⅳ) coupling for benzyl alcohol electrooxidation Co(Cu)0.5OxHy 微立方体中的非凡 d-d 杂化促进了 PhCH2O*-Co(Ⅳ) 偶联用于苯甲醇电氧化反应
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-15 DOI: 10.1016/j.apcatb.2024.123739
Lei Huang , Xiongchao Lin , Ke Zhang , Jun Zhang , Caihong Wang , Sijian Qu , Yonggang Wang
{"title":"Extraordinary d–d hybridization in Co(Cu)0.5OxHy microcubes facilitates PhCH2O* –Co(Ⅳ) coupling for benzyl alcohol electrooxidation","authors":"Lei Huang ,&nbsp;Xiongchao Lin ,&nbsp;Ke Zhang ,&nbsp;Jun Zhang ,&nbsp;Caihong Wang ,&nbsp;Sijian Qu ,&nbsp;Yonggang Wang","doi":"10.1016/j.apcatb.2024.123739","DOIUrl":"10.1016/j.apcatb.2024.123739","url":null,"abstract":"<div><p>A series of bimetallic hydroxides Co(M)<sub>0.5</sub>O<sub>x</sub>H<sub>y</sub><span> (M = Cu, Ni, Mn, Zn) were fabricated for the benzyl alcohol oxidation reaction (BAOR). The active origin and synergistic effect of bimetallic electrocatalysts were adequately deciphered. The reaction was found be principally initiated from the sequential oxidation of Co</span><sup>2+</sup> (i.e., Co<sup>2+</sup> to Co<sup>3+</sup> to Co<sup>4+</sup>), followed by the spontaneous proton–coupled electron transfer (PCET) process between Co<sup>4+</sup><span> and benzyl alcohol (BA) molecules. Besides, the adsorption free energy of BA molecules on Co(Cu)</span><sub>0.5</sub>O<sub>x</sub>H<sub>y</sub><span> was successfully optimized by Cu doping owing to the extraordinary d–d orbital hybridization between Co and Cu atom. As a result, an extra high conversion rate (95.3%) of BA and selectivity (98.2%) of benzoic acid were achieved under 0.5 V vs. Hg/HgO. These insights are essential for a comprehensive understanding of the BAOR mechanism and the design of Co–based catalysts.</span></p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139476897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-performance, stable buffer-layer-free La0.9Sr0.1Ga0.8Mg0.2O3 electrolyte-supported solid oxide cell with a nanostructured nickel-based hydrogen electrode 采用纳米结构镍基氢电极的高性能、稳定的无缓冲层 La0.9Sr0.1Ga0.8Mg0.2O3 电解质支撑固体氧化物电池
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-15 DOI: 10.1016/j.apcatb.2024.123742
Jiaqi Qian, Changgen Lin, Zhiyi Chen, Jiongyuan Huang, Na Ai, San Ping Jiang, Xiaoliang Zhou, Xin Wang, Yanqun Shao, Kongfa Chen
{"title":"High-performance, stable buffer-layer-free La0.9Sr0.1Ga0.8Mg0.2O3 electrolyte-supported solid oxide cell with a nanostructured nickel-based hydrogen electrode","authors":"Jiaqi Qian, Changgen Lin, Zhiyi Chen, Jiongyuan Huang, Na Ai, San Ping Jiang, Xiaoliang Zhou, Xin Wang, Yanqun Shao, Kongfa Chen","doi":"10.1016/j.apcatb.2024.123742","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.123742","url":null,"abstract":"<p>La<sub>0.9</sub>Sr<sub>0.1</sub>Ga<sub>0.8</sub>Mg<sub>0.2</sub>O<sub>3</sub> (LSGM) with an extraordinary oxygen-ion conductivity has been extensively studied as an electrolyte material for intermediate temperature solid oxide cells (SOCs). However, the conventional high-temperature sintering process of electrodes results in detrimental reaction between LSGM and Ni-based hydrogen electrode and microstructural coarsening of the electrode. Herein, a buffer-layer-free LSGM electrolyte-supported single cell with a nanostructured Ni-Gd<sub>0.1</sub>Ce<sub>0.9</sub>O<sub>1.95</sub> (GDC) electrode is developed using a sintering-free fabrication approach. The cell exhibits a peak power density of 1.23<!-- --> <!-- -->W<!-- --> <!-- -->cm<sup>−2</sup> at 800 °C and an electrolysis current density of 1.85<!-- --> <!-- -->A<!-- --> <!-- -->cm<sup>−2</sup> at 1.5<!-- --> <!-- -->V with excellent operating stability. The good performance and durability is owing to the synergistic effects of the elimination of elemental interdiffusion at the electrode/electrolyte interface, polarization induced <em>in situ</em> formation of hetero-interfaces between Ni-GDC and LSGM, and remarkable structural stability of Ni-GDC. This study provides an innovative means for the development of efficient and durable buffer-layer-free LSGM-supported SOCs.</p>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139475683","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficiently unbiased solar-to-ammonia conversion by photoelectrochemical Cu/C/Si-TiO2 tandems 通过光电化学 Cu/C/Si-TiO2 串联实现高效无偏的太阳能氨转化
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-14 DOI: 10.1016/j.apcatb.2024.123735
Jingjing Ding , Yanhong Lyu , Huaijuan Zhou , Bernt Johannessen , Xiaoran Zhang , Jianyun Zheng , San Ping Jiang , Shuangyin Wang
{"title":"Efficiently unbiased solar-to-ammonia conversion by photoelectrochemical Cu/C/Si-TiO2 tandems","authors":"Jingjing Ding ,&nbsp;Yanhong Lyu ,&nbsp;Huaijuan Zhou ,&nbsp;Bernt Johannessen ,&nbsp;Xiaoran Zhang ,&nbsp;Jianyun Zheng ,&nbsp;San Ping Jiang ,&nbsp;Shuangyin Wang","doi":"10.1016/j.apcatb.2024.123735","DOIUrl":"10.1016/j.apcatb.2024.123735","url":null,"abstract":"<div><p>Photoelectrochemical nitrate reduction reaction (PEC NO<sub>3</sub>RR) is of interest as a promising route to directly realizing the solar-to-ammonia (NH<sub>3</sub>) conversion but the limited efficiency and high applied bias voltage hamper its commercial prospects. Here, we report a bias-free photoelectrochemical cell for PEC NO<sub>3</sub>RR in aqueous conditions, achieving a substantial NH<sub>3</sub> yield rate of 13.1 μmol·h<sup>−1</sup>·cm<sup>−2</sup>, high faradaic efficiency of 93.8%, and recorded solar-to-NH<sub>3</sub> conversion of ∼1.5% under 1 sun illumination. A hierarchical-structured Si-based photocathode with Cu<sup>+</sup>/Cu<sup>2+</sup><span>-containing Cu nanoparticles cocatalysts achieves a highly efficient PEC NO</span><sub>3</sub>RR with NH<sub>3</sub> yield rate of 115.3 μmol·h<sup>−1</sup>·cm<sup>−2</sup><span> in a three-electrode system. Integrating operando characterizations and systematic PEC measurements, the formation of Lewis acid sites on Cu nanoparticles by accepting the photoinduced electrons is the dominant factor for facilitating the absorption and hydrogenation of nitrate. This work will guide the development of a robust, high-performance, and unbiased PEC device for sustainable solar-to-NH</span><sub>3</sub>/other fuels conversion.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139460322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Facilely tunable dodecahedral polyoxometalate framework loaded with mono- or bimetallic sites for efficient photocatalytic CO2 reduction 十二面体 POM 框架负载单金属或双金属位点,可轻松调谐,用于高效光催化还原 CO2
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-14 DOI: 10.1016/j.apcatb.2024.123733
Bonan Li , Mengxue Chen , Qiyu Hu , Jiayu Zhu , Xu Yang , Zhexu Li , Chunlian Hu , Yuanyuan Li , Ping Ni , Yong Ding
{"title":"Facilely tunable dodecahedral polyoxometalate framework loaded with mono- or bimetallic sites for efficient photocatalytic CO2 reduction","authors":"Bonan Li ,&nbsp;Mengxue Chen ,&nbsp;Qiyu Hu ,&nbsp;Jiayu Zhu ,&nbsp;Xu Yang ,&nbsp;Zhexu Li ,&nbsp;Chunlian Hu ,&nbsp;Yuanyuan Li ,&nbsp;Ping Ni ,&nbsp;Yong Ding","doi":"10.1016/j.apcatb.2024.123733","DOIUrl":"10.1016/j.apcatb.2024.123733","url":null,"abstract":"<div><p>Utilizing solar energy to drive the conversion of CO<sub>2</sub> into high-value chemicals emerged as a promising approach to decrease CO<sub>2</sub> emission. Yolk-shell or hollow structure have drawn much attention for photocatalytic CO<sub>2</sub> reduction, owing to their efficient CO<sub>2</sub> trapping and more active sites exposing. In this study, we employed a simple method to regulate the morphological evolution of K<sub>3</sub>PW<sub>12</sub>O<sub>40</sub> dodecahedra. After annealing, mono-/bimetallic active species are homogeneously dispersed on K<sub>3</sub>PW<sub>12</sub>O<sub>40</sub> framework forming PW<sub>12</sub> @Co and PW<sub>12</sub> @CoNi, which exhibit good CO production rates of 11.2 and 15.1 μmol/h, respectively, with selectivity of 90.7% and 92.6%. The differences in the activity and selectivity of CO<sub>2</sub>RR are attributed to the morphology variations of POM and the influence of mono-/bimetallic species. These results are confirmed through the analysis of SEM, TEM, N<sub>2</sub> and CO<sub>2</sub> adsorption/desorption, PL, EIS and SPV characterizations. In-situ DRIFTS and DFT provide further support for the formation and transformation of intermediate products.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139460214","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A novel biomass gasification process for the generation of inherently separated syngas using the concept of chemical looping technology 利用化学循环技术概念生成固有分离合成气的新型生物质气化工艺
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-13 DOI: 10.1016/j.apcatb.2024.123729
Haochen Sun , Zhiqing Wang , Hengyang Miao , Zheyu Liu , Jiejie Huang , Jin Bai , Chengmeng Chen , Yitian Fang
{"title":"A novel biomass gasification process for the generation of inherently separated syngas using the concept of chemical looping technology","authors":"Haochen Sun ,&nbsp;Zhiqing Wang ,&nbsp;Hengyang Miao ,&nbsp;Zheyu Liu ,&nbsp;Jiejie Huang ,&nbsp;Jin Bai ,&nbsp;Chengmeng Chen ,&nbsp;Yitian Fang","doi":"10.1016/j.apcatb.2024.123729","DOIUrl":"10.1016/j.apcatb.2024.123729","url":null,"abstract":"<div><p><span>Biomass-based hydrogen generation has been showing a potential prospect in solving the global environment and energy challenges. This study introduces a novel chemical looping system, known as chemical looping partial oxidation and hydrogen generation (CLPH) process, which can generate inherently separated syngas from biomass, thus presenting a good application prospect. The feasibility of this system and the selection of appropriate oxygen carriers (OCs), which were the key to the success of this system, were investigated in this work. Four MFe</span><sub>2</sub>O<sub>4</sub> (M=Ni, Co, Ca, Ba) OCs were chosen according to the modified Ellingham diagram, and their performances as well as the reaction pathway of BaFe<sub>2</sub>O<sub>4</sub> and C were comprehensively investigated. The results show that all OCs exhibit a good solid-solid reactivity, but the CO selectivity of CaFe<sub>2</sub>O<sub>4</sub> and BaFe<sub>2</sub>O<sub>4</sub> (around 60%) are higher than that of CoFe<sub>2</sub>O<sub>4</sub> and NiFe<sub>2</sub>O<sub>4</sub> (around 20%). Additionally, the cycle performance of CaFe<sub>2</sub>O<sub>4</sub> is worse than that of BaFe<sub>2</sub>O<sub>4</sub>, which is owing to the poor self-healing property. Thus, BaFe<sub>2</sub>O<sub>4</sub> was chosen as the ideal OC for the CLPH process. A successful biomass gasification process for the generation of inherently separated syngas was developed, achieving a carbon conversion rate of 93%, CO selectivity of ≥ 60%, wonderful hydrogen yield of ≥ 1700 mL/g·biomass char and hydrogen purity of ≥ 94% over 5 cycles.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":22.1,"publicationDate":"2024-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139460320","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling the role of catalytically active MXene supports in enhancing the performance and durability of cobalt oxygen evolution reaction catalysts for anion exchange membrane water electrolyzers 揭示催化活性 MXene 支持物在提高阴离子交换膜水电解槽钴氧进化反应催化剂的性能和耐用性方面的作用
IF 22.1 1区 化学
Applied Catalysis B: Environmental Pub Date : 2024-01-13 DOI: 10.1016/j.apcatb.2024.123731
Young Sang Park , Ari Chae , Gwan Hyun Choi , Swetarekha Ram , Seung-Cheol Lee , Satadeep Bhattacharjee , Jiyoon Jung , Hyo Sang Jeon , Cheol-Hee Ahn , Seung Sang Hwang , Dong-Yeun Koh , Insik In , Taegon Oh , Seon Joon Kim , Chong Min Koo , Albert S. Lee
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