Lizbeth Moreno Bravo, Frederic C. Meunier, Jan Kopyscinski
{"title":"Rare earth oxide promoted Ru/Al2O3 dual function materials for CO2 capture and methanation: An operando DRIFTS and TGA study","authors":"Lizbeth Moreno Bravo, Frederic C. Meunier, Jan Kopyscinski","doi":"10.1016/j.apcatb.2024.124591","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124591","url":null,"abstract":"Dual-function materials (DFMs) combine sorbent and catalytic components to perform selective CO capture and subsequent hydrogenation. This study explores the performance of rare-earth oxides (REOs) as CO adsorption sites on Ru/AlO. REOs increase CO uptake by upwards of +60 % by enhancing the overall catalyst surface basicity and favoring metal–support interactions. Thermogravimetric analysis during CO adsorption-hydrogenation cycles exhibited significant catalytic activity and enhanced stability of Ru-REO/AlO at temperatures as low as 200 °C. This leads to methane production of 50–85 µmol g, surpassing recently reported values obtained for alkali and alkali-earth promoted Ru-based materials operated at 250 °C. The highest performing studied DFM, RuNdO/AlO, achieved 85 % CO capture efficiency and steadily produced methane in cyclic operation (+120 % CO uptake relative to Ru/AlO). DRIFTS revealed that the dominant mechanism for methane formation is the hydrogenation of ruthenium carbonyls, which are stabilized by REOs. Upon CO exposure, surface carbonates and bicarbonate species form more abundantly on DFMs than on Ru/AlO. This confirms that REOs enhance the adsorption and retention of carbonates, which generate additional promoter-related reaction pathways during low-temperature hydrogenation. These findings are crucial in the advancement of sustainable, wider operation range carbon capture and utilization technologies.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"5 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142250054","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ling-Wei Wei, Shou-Heng Liu, Van-Can Nguyen, Meng-Wei Zheng, Hong Paul Wang
{"title":"Visible-light driven O2-to-H2O2 synchronized activation of peroxymonosulfate in Z-scheme photocatalytic fuel cell for wastewater purification with power generation","authors":"Ling-Wei Wei, Shou-Heng Liu, Van-Can Nguyen, Meng-Wei Zheng, Hong Paul Wang","doi":"10.1016/j.apcatb.2024.124594","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124594","url":null,"abstract":"Antibiotics are recognized as emerging contaminants with non-biodegradation, complex structures, and abundant chemical energy, which are difficult to treat and recover energy through traditional wastewater treatment processes. A Z-scheme photocatalytic fuel cell (PFC) system, comprising CN and CuO/CuO dual-photoelectrodes, has been developed for simultaneous power generation and degradation of antibiotics, such as berberine hydrochloride (BH). Especially, the CN with its suitable energy potential for peroxymonosulfate (PMS) activation is synchronized with CuO/CuO, resulting in enhancing the performance of PFC system. Moreover, the interaction between PMS and Cu(I)/Cu(II) active sites on the photocathode can enhance the formation of highly reactive species (HRS) in the PFC-PMS system, thereby improving photocatalytic oxidation performance. Under visible-light illumination for 120 min, PFC-PMS system can rapidly and effectively oxidize BH (ca. 99.2 %, = 0.0039 min) with simultaneous power generation (0.018 mW cm). This approach presents a promising approach for both water cleanup and energy reuse applications.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"75 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249994","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"La-exacerbated lattice distortion of high entropy alloys for enhanced electrocatalytic water splitting","authors":"Zhen-Long Wang, Gao-Yuan Huang, Guan-Rong Zhu, Huan-Chuan Hu, Cong Li, Xue-Han Guan, Hai-Bin Zhu","doi":"10.1016/j.apcatb.2024.124585","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124585","url":null,"abstract":"The complex active site configurations of high entropy alloys (HEAs) limit their performance optimization and wide applications. Herein, we report a FeCoNiMnRuLa/CNT catalyst for efficient electrocatalytic water splitting by introducing La to break the lattice ordering of FeCoNiMnRu. The introduction of La reduces the number of unpaired electrons in FeCoNiMnRu, which in turn accelerates the transition of singlet state oxygen-containing intermediate to triplet state oxygen. The DFT results verify that the lattice distortion exacerbated by La alters the d-orbital electronic configuration of FeCoNiMnRu, so that Fe and Ni play an important role in the critical adsorption of *OH in the OER as well as *HO in the HER, and Ru, Co, and Mn provide a strong safeguard for the desorption of oxygen-containing intermediates, thereby retaining excellent activity and stability during water decomposition. Our work showcases that the incorporation of rare earth elements opens new opportunities to improve the performance of HEAs.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"2 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142250059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lu Lin, Yongjian Zeng, Suyu Zhang, Di Hu, Zhiwei Jiang, Guoqing Guan, Kai Yan
{"title":"Tuning ligand-vacancies in Pd-UiO-66 to boost biofuel production from 5-hydroxymethylfurfural hydrodeoxygenation","authors":"Lu Lin, Yongjian Zeng, Suyu Zhang, Di Hu, Zhiwei Jiang, Guoqing Guan, Kai Yan","doi":"10.1016/j.apcatb.2024.124592","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124592","url":null,"abstract":"The hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) to biofuel 2,5-dimethylfuran (DMF) serves as a vital reaction in biomass refineries. Herein, Pd-UiO-66 catalysts with controlled contents of ligand-vacancies were developed for the HMF-to-DMF conversion. Strikingly, a volcano-like relationship between defect level and HDO activity was obtained. The DMF yield was promoted ∼3 times, reaching 92.2 % at 160 °C and 15 bar H, which refers to a high-level turnover frequency value of 42.66 h among the reported candidates. The Pd-UiO-66 catalysts also afforded >80 % yield for the HDO of 5-methyl furfural, furfural, and vanillin. Besides, high HDO activity could be retained in five recycles. Manipulating the contents of ligand-vacancies was confirmed to create more Pd species and Bronsted acid sites, leading to remarkable performance. This work provides significant inspiration for tuning structural defects in MOFs to realize the efficient HDO of platform molecules in biomass valorization.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"53 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249993","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yunzhe Zheng, Xinhao Wang, Yudan Dong, Xiaoyu Wu, Donghua Xie, Yang Liu, Peng Zhou, Zhaokun Xiong, Chuan-Shu He, Bo Lai
{"title":"Overlooked role of boron precursors in tuning engineered zero-valent iron to activate peracetic acid for sustainable micropollutant oxidation","authors":"Yunzhe Zheng, Xinhao Wang, Yudan Dong, Xiaoyu Wu, Donghua Xie, Yang Liu, Peng Zhou, Zhaokun Xiong, Chuan-Shu He, Bo Lai","doi":"10.1016/j.apcatb.2024.124580","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124580","url":null,"abstract":"This work comprehensively investigated how the characteristics of boron (B) precursors affect the catalytic activity of microscale zero-valent iron (mZVI) towards peracetic acid (PAA) activation for micropollutant degradation. Three boron precursors were introduced into mZVI by ball milling with their physical-chemical properties carefully characterized, and their ability to activate PAA comprehensively evaluated via sulfamethoxazole (SMX) oxidation efficiency. It’s found that BO-ZVI demonstrated the highest capability to activate PAA for SMX degradation, with 2 ∼ 3 times higher than NaBO-ZVI and HBO-ZVI. Specially, B precursors regulate the ability of mZVI to activate PAA via the following two aspects: (1) affecting the formation and content of FeB to accelerate Fe(II) regeneration; (2) increasing the hydrophilicity of the iron particles and the affinity of B-ZVI for binding PAA to different extent. This study highlights the important role of boron precursors in tuning engineered mZVI to initiate Fenton-like process for water purification.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"40 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249997","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Highly crystalline benzothiadiazole covalent organic framework for enhanced Cr(VI) photocatalytic reduction by constructing donor-acceptor structure","authors":"Chen Wang, Wen Lu, Wenhui Song, Zhixiong Zhang, Chengde Xie, Yu Li, Jianjun Wang","doi":"10.1016/j.apcatb.2024.124583","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124583","url":null,"abstract":"Covalent organic frameworks (COFs) have gained significant attention in environmental remediation. In this paper, we synthesized two sp carbon-conjugated COFs (HDU-107 and HDU-108) using [1,1′:4′,1''-terphenyl]-4,4''-dicarbonitrile and 2,2′-(benzo[][1,2,5]thiadiazole-4,7-diylbis(4,1-phenylene))diacetonitrile as the core, and benzo[1,2-b:3,4-b′:5,6-b″]trithiophene-2,5,8-tricarbaldehyde as the linker, for efficient photocatalytic reduction of Chromium (VI) (Cr(VI)). HDU-108 successfully constructed an electron donor-acceptor (D-A) structure using electron-rich thiophene as the electron donor and benzothiadiazole as the acceptor, exhibiting excellent photocatalytic ability due to its structure, which facilitated the spatial separation of charge carriers and reduced charge complexation. This ability was far superior to that of HDU-107. For 10 mg of HDU-108, the efficiency of Cr(VI) reduction in 120 minutes was more than 99.9 %. And the cycle experiments confirmed its good reusability and stability. e played a dominant role in the photoreduction of Cr(VI). Moreover, density-functional theory (DFT) simulations indicated that constructing D-A structures was an effective strategy for modulating photocatalytic activity. The charge separation was triggered by the polarization of the electron-rich BTT nucleus to the local charge density, while the cyanine conjugation provided the active center to concentrate the electronegativity. In conclusion, HDU-108, is expected to be a highly efficient photocatalytic material for environmental remediation.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"2677 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Bi2SiO5 nanosheets as piezo-photocatalyst for efficient degradation of 2,4-Dichlorophenol","authors":"Hangyu Shi, Yifu Li, Lishan Zhang, Guoguan Liu, Qian Zhang, Xuan Ru, Shan Zhong","doi":"10.1016/j.apcatb.2024.124581","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124581","url":null,"abstract":"Piezo-photocatalysis is an effective solution for degrading organic pollutants. In this study, BiSiO nanosheets are successfully synthesized via a one-step hydrothermal method. The piezo-photocatalytic degrading mechanisms of 2,4-Dichlorophenol (2,4-DCP) on BiSiO nanosheets are thoroughly investigated through the integration of experimental study and density functional theory (DFT) calculations. Experimental results revealed outstanding piezoelectric properties for BiSiO nanosheets with a piezoelectric coefficient of 250 pC/N, outperforming previously reported piezo-photocatalysts. The degradation rate constant of 2,4-DCP on BiSiO nanosheets reached 0.0891 min by piezo-photocatalysis, which is 17 and 1.8 times higher than that by solitary photo- and piezo-catalysis, respectively. Furthermore, DFT calculations for BiSiO explain the crucial role of piezoelectric effects in bending its band structure, regulating photogenerated carrier behaviors, and promoting reactive oxygen species (ROS) generation. Finally, the degradation pathways of 2,4-DCP on BiSiO nanosheets were revealed with details. The results of this study offer valuable insights for water treatment with piezo-photocatalysis.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"15 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249739","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Selective switching hydrogenation products of 5-hydroxymethylfurfural at high substrate concentrations by regulating Pd-MgO interactions","authors":"Mingxin Lv, Liyuan Huai, Guoxin Chen, Xi Zhao, Chunlin Chen, Shenghu Zhou, Jian Zhang","doi":"10.1016/j.apcatb.2024.124578","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124578","url":null,"abstract":"Controlling the selective activation of one or some functional groups as desired is still a challenge in hydrogenation, especially at high substrate concentrations. Herein, Pd-MgO interfaces over AlO were finely regulated for efficiently selective hydrogenation of furan ring in 5-hydroxymethylfurfural (HMF) to produce 5-hydroxymethyltetrahydro-2-furaldehyde (5-HMTHFF) or total hydrogenation to 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF), also inhibiting side reaction. The Pd-MgO/AlO with 12.0 wt% of MgO selectively hydrogenates the furan rings with a 5-HMTHFF yield of 82.4 % while that with 2.0 wt% of MgO totally hydrogenates HMF with a DHMTHF yield of 96.2 % at high substrate concentrations (400 mM). Characterizations and DFT calculations demonstrated that oligomeric MgO species suppress the agglomeration of Pd nanoparticles and strengthen HMF adsorption, consequently promoting total hydrogenation. Furthermore, Pd-MgO sites between the crystallized MgO and Pd metal favored tilted adsorption on the interface and weakened the activation of the CO bond, consequently selectively producing 5-HMTHFF.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"2 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249998","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bohua Sun, Qianqian Li, Guijin Su, Maoyong Song, Chunyan Ma, Jiaxin Pang, Xu Zhao, Jing Meng, Bin Shi
{"title":"Sustainable and efficient catalytic oxidation of chlorinated volatile organic compounds over Ru-loaded facet-engineered {201}-TiO2 catalyst with tuned defects","authors":"Bohua Sun, Qianqian Li, Guijin Su, Maoyong Song, Chunyan Ma, Jiaxin Pang, Xu Zhao, Jing Meng, Bin Shi","doi":"10.1016/j.apcatb.2024.124582","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124582","url":null,"abstract":"Sustainable and efficient catalytic oxidation of chlorinated volatile organic compounds (CVOCs) poses an enduring challenge. This bottleneck arises from the limited catalytic activity of redox reactions and chlorine desorption, causing catalyst deactivation and secondary pollution. Herein, our sound strategy involves Ru-loaded facet-engineered {201}-TiO with tuned defects, thereby boosting its reactivity. Comprehensive characterizations and DFT calculation manifested that Ru/{201}-TiO, with abundant oxygen vacancies, Ti defects, and robust metal-support interaction, enabled flexible electron transfer to activate O and the dissociation of HO, thus facilitating the continuous generation of reactive oxygen species (ROS), such as •O and hydroxyl species. These ROS effectively enhance chlorine desorption and chlorobenzene deep oxidation. Ru/{201}-TiO exhibited superior reactivity for chlorobenzene degradation, with an apparent activation energy (Ea) of 31.0 KJ/mol and 100 % chlorobenzene conversion in a 1000-min stability test, even with HO introduction. Ru/{201}-TiO produced 2.2–3.1 times fewer small-molecule chlorinated byproducts than Ru/{101}-TiO, with no polychlorinated benzenes detected.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"9 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249995","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaoling Ren, Honghui Ou, Wei Liu, Yang Lv, Aofei Xu, Zhiwei Ren, Bolun Yang, Guidong Yang
{"title":"New Lewis acidic ionic liquid coupled carbon shell coated defective WO3 for efficient photocatalytic N2 reduction","authors":"Xiaoling Ren, Honghui Ou, Wei Liu, Yang Lv, Aofei Xu, Zhiwei Ren, Bolun Yang, Guidong Yang","doi":"10.1016/j.apcatb.2024.124579","DOIUrl":"https://doi.org/10.1016/j.apcatb.2024.124579","url":null,"abstract":"Herein, a new strategy to enhance the nitrogen concentration around the photocatalyst for photocatalytic nitrogen reduction was proposed. And new type of acidic ionic liquid (IL) coupled defective tungsten oxide coated with carbon shell (W@C) was designed and synthesized. The results show that the interaction force between IL and nitrogen is stronger than that between water and nitrogen, which increases the concentration of nitrogen around the tungsten oxide catalyst. In addition, the carbon shell with a hollow structure has a molecular enrichment effect, which can effectively achieve nitrogen enrichment and reduce IL escape. Finally, the ammonia synthesis performance of acidic IL coupled W@C is 52.6 μmol g h, which is about 9 times and 2 times of tungsten oxide and W@C sample, respectively. This work fully reveals the importance of designing the catalyst structure reasonably and increasing the nitrogen concentration around the catalyst to improve the photocatalytic nitrogen reduction performance.","PeriodicalId":516528,"journal":{"name":"Applied Catalysis B: Environment and Energy","volume":"16 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142250049","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}