Chinese Journal of Catalysis最新文献_第8页

Self-supported film catalyst integrated with multifunctional carbon nanotubes and Ni-Ni(OH)2 heterostructure for promoted hydrogen evolution 集成了多功能碳纳米管和 Ni-Ni(OH)2 异质结构的自支撑薄膜催化剂用于促进氢气进化

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI: 10.1016/S1872-2067(24)60057-4

Wancheng Zhao , Jiapeng Ma , Dong Tian , Baotao Kang , Fangquan Xia , Jing Cheng , Yajun Wu , Mengyao Wang , Gang Wu

{"title":"Self-supported film catalyst integrated with multifunctional carbon nanotubes and Ni-Ni(OH)2 heterostructure for promoted hydrogen evolution","authors":"Wancheng Zhao , Jiapeng Ma , Dong Tian , Baotao Kang , Fangquan Xia , Jing Cheng , Yajun Wu , Mengyao Wang , Gang Wu","doi":"10.1016/S1872-2067(24)60057-4","DOIUrl":"10.1016/S1872-2067(24)60057-4","url":null,"abstract":"<div>In order to reduce energy consumption in water electrolysis, it is of great importance to design active and stable electrocatalysts for hydrogen evolution reaction (HER) in alkaline solution, especially based on earth-abundant metal. Here we integrate carbon nanotubes (CNTs) and Ni-Ni(OH)2 heterostructure multifunctional components to design a self-supported 3D CNTs-Ni-Ni(OH)2 catalyst for HER by composite deposition and subsequent in-situ oxidation. In alkaline solution, this designed CNTs-Ni-Ni(OH)2 catalyst exhibits 0 mV onset overpotential, and overpotentials of 65 mV and 109 mV at 10 and 50 mA/cm2 respectively. Electrochemical measurements, characterizations, and simulation results attribute the outstanding performance to the incorporation of CNTs and heterostructure. CNTs induce the formation 3D catalytic surface, enhance electrochemical active surface area, and more importantly weaken the adsorption of H. Moreover, the formation of heterostructure, especially reversible Ni(OH)2, supplies active sites and adjusts the adsorption strength of H atom to an optimal value. CNTs and heterostructure synergistically facilitate water adsorption, promote water dissociation, and accelerate H2 desorption. Significantly, integration of multifunctional components supplies a distinct strategy for development of cost-effective electrocatalyst with outstanding performance.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"62 ","pages":"Pages 287-295"},"PeriodicalIF":15.7,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141729642","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

Photo-thermal cooperation for the conversion of CO2 and CH4 with H2O to C2 oxygenates over SrTiOx supported CuCo 在 SrTiOx 支持的 CuCo 上利用光热合作将 CO2 和 CH4 与 H2O 转化为 C2 氧酸盐

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60026-4

Yanru Zhu , Zhijun Zhang , Jian Zhang , Shuangjiang Jiang , Zhe An , Hongyan Song , Xin Shu , Wei Xi , Lirong Zheng , Jing He

{"title":"Photo-thermal cooperation for the conversion of CO2 and CH4 with H2O to C2 oxygenates over SrTiOx supported CuCo","authors":"Yanru Zhu , Zhijun Zhang , Jian Zhang , Shuangjiang Jiang , Zhe An , Hongyan Song , Xin Shu , Wei Xi , Lirong Zheng , Jing He","doi":"10.1016/S1872-2067(24)60026-4","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60026-4","url":null,"abstract":"<div>Photosynthesis is a potential strategy to enable endergonic process that usually needs high-temperature in thermochemistry to supply the energy for inert-bond activation and/or strong endothermic reaction. The conversion of CO2 into value-added C2-oxygenates is a promising process to realize artificial photosynthesis, but suffers from relatively lower efficiency due to complex multi-electron (≥ 10) transfer processes and sluggish kinetics of C–C coupling. This work proposes an all-new H2O-promoted strategy for efficient production of C2 oxygenates from the concurrent activation and subsequent co-conversion of CO2 with CH4 under photo-thermal cooperation, in which photocatalytic H2O-splitting derived active hydrogen species for CO2 activation, and concomitant active oxygen species for CH4 activation. A formation rate of as high as 2.05 mmol g−1 h−1 for C2-oxygenates (CH3CHO and CH3CH2OH) in a selectivity of > 86% has been afforded over SrTiOx supported CuCo under 200 °C and ultraviolet-visible illumination. It has been revealed that SrTiOx drives photocatalytic H2O-splitting under the excitation primary from ultraviolet light, paired CuI/Cu0 sites promote the formation of *CHxO intermediate from CO2, Co sites conduct CH4-to-*CH3, and C–C coupling of *CHxO and *CH3 on adjacent Cu-Co facilitates the generation of C2-oxygenates.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 164-178"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606577","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

Constructing amorphous/crystalline NiFe-MOF@NiS heterojunction catalysts for enhanced water/seawater oxidation at large current density 构建非晶/晶态 NiFe-MOF@NiS 异质结催化剂，在大电流密度下增强水/海水氧化能力

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60030-6

Xianbiao Hou , Chen Yu , Tengjia Ni , Shucong Zhang, Jian Zhou, Shuixing Dai, Lei Chu, Minghua Huang

{"title":"Constructing amorphous/crystalline NiFe-MOF@NiS heterojunction catalysts for enhanced water/seawater oxidation at large current density","authors":"Xianbiao Hou , Chen Yu , Tengjia Ni , Shucong Zhang, Jian Zhou, Shuixing Dai, Lei Chu, Minghua Huang","doi":"10.1016/S1872-2067(24)60030-6","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60030-6","url":null,"abstract":"<div>Developing metal-organic frameworks (MOF) based catalysts with high activity and chlorine corrosion resistance is of paramount importance for seawater oxidation at large current density. Herein, we report a heterogeneous structure coupling NiFe-MOF nanoparticles with NiS nanosheets onto Ni foam (denoted as the NiFe-MOF@NiS/NF) via the mild strategy involving sulfur-modified corrosion and electrodeposition treatment. The constructed amorphous/crystalline interfaces could not only facilitate the adequate infiltration of electrolyte and release of O2 bubbles at large current densities, but also significantly improve the charge transfer from NiFe-MOF to NiS and the adsorption/desorption capacity of oxygen intermediates. Intriguingly, during oxygen evolution reaction process, the sulfate film formed by the self-reconstruction could remarkably inhibit the adsorption of Cl– ions on the catalyst surface in the seawater electrolytes. Benefiting from the robust corrosion resistance, unique amorphous/crystalline interfaces, and the charge redistribution, the well-designed NiFe-MOF@NiS/NF exhibits the low overpotential of 346 and 355 mV under a high current density of 500 mA cm−2 in alkaline water and seawater electrolytes, respectively. More importantly, the as-fabricated NiFe-MOF@NiS/NF demonstrates prolonged stability and durability, lasting over 600 h at a current density of 100 mA cm−2 in both electrolytes. This study enriches the understanding of electronic structure modulation and chlorine corrosion resistance in seawater, providing broad prospects for designing advanced MOF-based catalysts.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 192-204"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606582","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

Enhancement of H2O2 generation rate in porphyrin photocatalysts via crystal facets regulation to create strong internal electric field 通过调节晶面以产生强内电场，提高卟啉光催化剂中 H2O2 的生成率

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60039-2

Yunhang Shao , Yaning Zhang , Chaofeng Chen , Shuai Dou , Yang Lou , Yuming Dong , Yongfa Zhu , Chengsi Pan

{"title":"Enhancement of H2O2 generation rate in porphyrin photocatalysts via crystal facets regulation to create strong internal electric field","authors":"Yunhang Shao , Yaning Zhang , Chaofeng Chen , Shuai Dou , Yang Lou , Yuming Dong , Yongfa Zhu , Chengsi Pan","doi":"10.1016/S1872-2067(24)60039-2","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60039-2","url":null,"abstract":"<div>Three TCPP porphyrin-based nanosheet photocatalysts with exposed (400), (022), and (020) planes were synthesized using a dissolution-recrystallization method in a mixture of water and tetrahydrofuran (THF), methanol (MeOH), and ethylene glycol (EG). The TCPP photocatalyst with the exposed (400) surface exhibited the highest H2O2 production rate of 29.33 mmol L−1 h−1 g−1 from only H2O and O2, surpassing the rates observed for ones with exposed (022) and (020) surfaces by factors of 2.7 and 4.1, respectively, and 1.3 times as that of the reported TCPP prepared by a base/acid self-assembling method. This enhancement can be attributed to the strong internal electric field and high carboxyl group content on the (400) surface, which hindered rapid charge recombination and facilitated challenging water oxidation. Hence, successful manipulation of porphyrin exposure to robust IEF planes enhances the photocatalytic activity of the system and provides valuable insights for the design and development of more efficient organic photocatalysts.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 205-214"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606583","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

Recent advances in metal titanate-based piezocatalysts: Enhancing catalytic performance through improved piezoelectric properties and regulated carrier transport 金属钛酸盐基压电催化剂的最新进展：通过改善压电特性和调节载流子传输提高催化性能

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(23)64635-2

Kaiqi Wang, Yiming He

{"title":"Recent advances in metal titanate-based piezocatalysts: Enhancing catalytic performance through improved piezoelectric properties and regulated carrier transport","authors":"Kaiqi Wang, Yiming He","doi":"10.1016/S1872-2067(23)64635-2","DOIUrl":"https://doi.org/10.1016/S1872-2067(23)64635-2","url":null,"abstract":"<div>Piezocatalysis, as an emerging technology, holds the promise for providing sustainable solutions to environmental remediation and energy management through mechanical energy utilization. Metal titanates (MTs) are well-known for their outstanding piezoelectric response, positioning them as the primary candidates for catalysts in this field. Moreover, their eco-friendly and cost-effective attributes have made them the focus of considerable attention among researchers. However, the insufficient piezocatalytic activity continues to constrain the practical application of MTs. Confronted with suboptimal energy conversion efficiency, enhancing the response to mechanical energy and reducing the subsequent conversion losses are pivotal for improving the piezocatalytic performance. This review commences with the classification and introduction of various MTs relevant to the field of piezocatalysis. Subsequently, the main methods for preparing MTs are presented. Particularly, the design strategies of MTs with excellent piezocatalytic properties are discussed from the perspectives of improving piezoelectric properties and regulating carrier transport, including construction of morphotropic phase boundary, strain engineering, Curie point control, external field-induced polarization, oriented crystal growth, co-catalyst loading, carbon modification, and semiconductor heterostructure construction. Finally, comprehensive challenges to the development of piezocatalytic technology are presented to promote the rational design and practical application of piezocatalysts.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 111-134"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141607514","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

Mechanistic insights and the role of spatial confinement in catalytic dimethyl ether carbonylation over SSZ-13 zeolite SSZ-13沸石催化二甲醚羰基化的机理认识和空间限制作用

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60040-9

Xiaomin Zhang , Kai Cai , Ying Li , Ji Qi , Yue Wang , Yunduo Liu , Mei-Yan Wang , Shouying Huang , Xinbin Ma

{"title":"Mechanistic insights and the role of spatial confinement in catalytic dimethyl ether carbonylation over SSZ-13 zeolite","authors":"Xiaomin Zhang , Kai Cai , Ying Li , Ji Qi , Yue Wang , Yunduo Liu , Mei-Yan Wang , Shouying Huang , Xinbin Ma","doi":"10.1016/S1872-2067(24)60040-9","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60040-9","url":null,"abstract":"<div>The SSZ-13 zeolite, which exhibits typical CHA topology characterized by 8-membered ring (8-MR) channels, has shown potential for catalyzing dimethyl ether (DME) carbonylation. However, current studies have yet to provide a comprehensive analysis of its catalytic mechanisms. In this study, we investigated the mechanism of SSZ-13-catalyzed DME carbonylation and the role of spatial confinement in this reaction. By exploiting the differences in the radii of the metal ions, we selectively replaced Brønsted acid sites (BAS) within specific channels, as confirmed by quantitative acidity analysis. Combining the activity data and the dissociation energies of the reactants on the BAS within different rings, we found that both the main and side reactions of DME carbonylation occurred on the 8-MR BAS of SSZ-13. Furthermore, the exchange of ions of different radii highlighted the confinement effect of the pore space in the SSZ-13 zeolite. Characterization of the deposits in spent catalysts, along with theoretical insights, revealed that the reduced cage space adversely affects the stabilization of side reaction intermediates, which in turn mitigates side reactions and improves the selectivity toward methyl acetate. This study presents an effective approach to modulate the acid site distribution and spatial confinement and provides critical insights into the determinants of the catalytic performance of SSZ-13. These findings offer valuable guidance for the future design and optimization of zeolites, aiming to enhance their efficacy in catalytic applications.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 301-311"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606578","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

Phase engineering of Ru-based nanocatalysts for enhanced activity toward CO2 methanation 基于 Ru 的纳米催化剂的相工程，提高 CO2 甲烷化活性

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60055-0

Chongya Yang , Weijue Wang , Hongying Zhuo , Zheng Shen , Tianyu Zhang , Xiaofeng Yang , Yanqiang Huang

{"title":"Phase engineering of Ru-based nanocatalysts for enhanced activity toward CO2 methanation","authors":"Chongya Yang , Weijue Wang , Hongying Zhuo , Zheng Shen , Tianyu Zhang , Xiaofeng Yang , Yanqiang Huang","doi":"10.1016/S1872-2067(24)60055-0","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60055-0","url":null,"abstract":"<div>The catalytic behavior of metal nanocatalysts is intrinsically contingent on the diversity of their exposed surfaces, which can be substantially regulated through the phase engineering of metal nanoparticles. In this study, it is demonstrated that the face-centered cubic (fcc) phase Ru with a close-packed (111) surface presents superior catalytic activity towards CO2 methanation. This behavior is attributed to its enhanced capability toward CO2 chemisorption derived from its inherently high surface reactivity. Complete exposure of such surfaces was successfully achieved experimentally by the synthesis of icosahedral Ru metal nanoparticles, which exhibited remarkable performance for CO2 methanation with 5–8 times higher activity than its conventional hexagonal close-packed (hcp) counterpart when supported on inert supports. However, for the joined fcc-Ru nanoparticles in the fresh catalyst, an fcc- to hcp-phase transformation was observed at a relatively high temperature with the in situ characterizations, which resulted in metal agglomeration and led to catalyst deactivation. However, the CO2 conversion was still much higher than that of the hcp-phase Ru nanocatalysts, as the monodispersed particles could maintain their fcc phase. Our results demonstrate that phase engineering of Ru nanocatalysts is an effective strategy for a catalyst design with improved catalytic performance. However, the phase transformation could represent a latent instability of the catalysts, which should be considered for the further development of robust catalysts.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 226-236"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606585","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 multiple effects of MOF-derived TiO2 on Ti-Fe2O3 photoanodes for efficient and stable photoelectrochemical water oxidation 揭示 MOF 衍生 TiO2 对 Ti-Fe2O3 光阳极的多重影响，实现高效稳定的光电化学水氧化作用

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60005-7

Kaikai Ba , Yuʼnan Liu , Kai Zhang , Ping Wang , Yanhong Lin , Dejun Wang , Ziheng Li , Tengfeng Xie

{"title":"Unveiling the multiple effects of MOF-derived TiO2 on Ti-Fe2O3 photoanodes for efficient and stable photoelectrochemical water oxidation","authors":"Kaikai Ba , Yuʼnan Liu , Kai Zhang , Ping Wang , Yanhong Lin , Dejun Wang , Ziheng Li , Tengfeng Xie","doi":"10.1016/S1872-2067(24)60005-7","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60005-7","url":null,"abstract":"<div>α-Fe2O3 is a promising photoanode that is limited by its high surface charge recombination and slow water oxidation kinetics. In this study, we synthesized a TiO2 layer on Ti-Fe2O3 by annealing Ti-MOFs, followed by ZIF-67 as a co-catalyst, to fabricate a ZIF-67/TiO2/Ti-Fe2O3 photoanode for photoelectrochemical (PEC) water splitting. The systematic experimental and theoretical results revealed that the improvement in performance was due to multiple effects of the MOF-derived TiO2. This molecule not only passivates the acceptor surface states of Ti-Fe2O3, thereby reducing the number of surface recombination centers, but also acts as an electron barrier to promote charge separation in the Ti-Fe2O3 bulk. Moreover, MOF-derived TiO2 can dramatically reduce the energy barrier for the OER of Ti-Fe2O3, thus promoting the conversion of the intermediate *OH into *O. The synergistic improvement in the bulk and surface properties effectively enhanced the water oxidation performance of Ti-Fe2O3. The ZIF-67/TiO2/Ti-Fe2O3 photoanode exhibits a photocurrent density of up to 4.04 mA cm−2 at 1.23 V vs. RHE, which is 9.4 times as that of pure Ti-Fe2O3, and has long-term stability. Our work provides a feasible strategy for constructing efficient organic-inorganic hybrid photoelectrodes.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 179-191"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606613","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

Defect-induced in situ electron-metal-support interactions on MOFs accelerating Fe(III) reduction for high-efficiency Fenton reactions MOFs 上缺陷诱导的原位电子-金属-支撑相互作用可加速铁（III）还原，从而实现高效芬顿反应

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60047-1

Haifang Mao , Yang Liu , Zhenmin Xu , Zhenfeng Bian

{"title":"Defect-induced in situ electron-metal-support interactions on MOFs accelerating Fe(III) reduction for high-efficiency Fenton reactions","authors":"Haifang Mao , Yang Liu , Zhenmin Xu , Zhenfeng Bian","doi":"10.1016/S1872-2067(24)60047-1","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60047-1","url":null,"abstract":"<div>The inefficient reduction of Fe3+ and activation of H2O2 in the Fenton reaction severely limit its application in practical water treatment. In this study, we developed defective NH2-UiO-66 (d-NU) with coordinated unsaturated metal sites by adjusting the coordination configuration of Zr, creating a solid-liquid interface to facilitate Fe3+ reduction and the sustainable generation of •OH from H2O2 activation. The d-NU/Fe3+/H2O2/Vis system demonstrated highly efficient removal of various organic pollutants, with a rapid Fe2+ regeneration rate and exceptional stability over ten cycles. The degradation rate constant of d-NU (0.16112 min–1) was 11 times higher than that of NH2-UiO-66 (NU) (0.01466 min–1) without defects. Characterization combined with density functional calculations revealed that defects induced coordination unsaturation of the Zr sites, leading to in situ electron-metal-support interactions between Fe3+ and the support via Zr–O–Fe bridges. This accumulation of electrons from the unsaturated Zr sites enabled the adsorption of Fe3+ at the solid-liquid interface, promoting the formation of Fe2+ across a wide pH range with a reduced energy barrier. This study introduces a promising strategy for accelerating Fe3+ reduction in the solid-liquid interfacial Fenton process for the degradation of organic pollutants.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 247-258"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606581","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

Spontaneous dispersion of metallic nickel centers in inert metal substrate for the selective hydrogenation of carbon-carbon triple bonds 金属镍中心在惰性金属基底中的自发分散，用于选择性氢化碳-碳三键

IF 15.7 1区化学

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI: 10.1016/S1872-2067(24)60048-3

Xin Deng , Caiyan Zheng , Weijie Li , Jiamin Wang , Di Yang , Zhenpeng Hu , Landong Li

{"title":"Spontaneous dispersion of metallic nickel centers in inert metal substrate for the selective hydrogenation of carbon-carbon triple bonds","authors":"Xin Deng , Caiyan Zheng , Weijie Li , Jiamin Wang , Di Yang , Zhenpeng Hu , Landong Li","doi":"10.1016/S1872-2067(24)60048-3","DOIUrl":"https://doi.org/10.1016/S1872-2067(24)60048-3","url":null,"abstract":"<div>Single-site metal catalysts with maximal utilization of active centers and desired target product selectivity represent a hot research topic within the realms of both academic and industry. However, the synthetic strategy is generally complicated and requires the precise control of interplay between metal centers and supporting materials. Herein, a simple spontaneous dispersion and universal strategy are developed to construct all-metal catalyst systems containing isolated metallic centers utilizing the spontaneous dispersion behaviors of transition metal centers Ni in inert substrate (Al, Mg and Ti). Ni/Al and Ni/Mg show remarkable performances in the model reaction of acetylene semi-hydrogenation with state-of-the-art site-specific activity, high ethylene selectivity and good stability. Especially, Ni/Al is reported for the first time to be an eligible low-cost catalyst for the selective hydrogenation of carbon-carbon triple bonds, surpassing the benchmark Lindlar catalyst. The reaction mechanism of acetylene semi-hydrogenation over Ni/Al catalyst is well clarified via the combination of kinetic analyses, spectroscopy investigation and theoretical calculations. The innovative approach developed herein not only expands the synthetic strategies toward single-site metal catalysts but also holds promise for practical applications in diverse chemical transformations due to the intrinsic advantages of all-metal systems.</div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"61 ","pages":"Pages 259-268"},"PeriodicalIF":15.7,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141606587","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