Journal of Energy Chemistry最新文献_第6页

Interfacial engineering and rapid thermal crystallization of Sb2S3 photoanodes for enhanced photoelectrochemical performances Sb2S3光阳极的界面工程与快速热结晶研究

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-27 DOI: 10.1016/j.jechem.2025.04.044

Runfa Tan , Seo Yeong Hong , Yoo Jae Jeong , Seong Sik Shin , In Sun Cho

{"title":"Interfacial engineering and rapid thermal crystallization of Sb2S3 photoanodes for enhanced photoelectrochemical performances","authors":"Runfa Tan , Seo Yeong Hong , Yoo Jae Jeong , Seong Sik Shin , In Sun Cho","doi":"10.1016/j.jechem.2025.04.044","DOIUrl":"10.1016/j.jechem.2025.04.044","url":null,"abstract":"<div><div>Antimony sulfide (Sb<sub>2</sub>S<sub>3</sub>) is a promising material for photoelectrochemical (PEC) devices that generate green hydrogen from sunlight and water. In this study, we present a synthesis of high-performance Sb<sub>2</sub>S<sub>3</sub> photoanodes via an interface-engineered hydrothermal growth followed by rapid thermal annealing (RTA). A TiO<sub>2</sub> interfacial layer plays a crucial role in ensuring homogeneous precursor deposition, enhancing light absorption, and forming efficient heterojunctions with Sb<sub>2</sub>S<sub>3</sub>, thereby significantly improving charge separation and transport. RTA further improves crystallinity and interfacial contact, resulting in dense and uniform Sb<sub>2</sub>S<sub>3</sub> films with enlarged grains and fewer defects. The optimized Sb<sub>2</sub>S<sub>3</sub> photoanode achieves a photocurrent density of 2.51 mA/cm<sup>2</sup> at 1.23 V vs. the reversible hydrogen electrode (RHE), one of the highest reported for Sb<sub>2</sub>S<sub>3</sub> without additional catalysts or passivation layers. To overcome the limitations of oxygen evolution reaction (OER), we employ the iodide oxidation reaction (IOR) as an alternative, significantly lowering the overpotential and improving charge transfer kinetics. Consequently, it produces a record photocurrent density of 8.9 mA/cm<sup>2</sup> at 0.54 V vs. RHE. This work highlights the synergy between TiO<sub>2</sub> interfacial engineering, RTA-induced crystallization, and IOR-driven oxidation, offering a promising pathway for efficient and scalable PEC hydrogen production.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 417-426"},"PeriodicalIF":13.1,"publicationDate":"2025-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071134","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

Reasonable control of cut-off voltage to achieve stable lithium metal anode 合理控制截止电压，实现锂金属阳极稳定

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-27 DOI: 10.1016/j.jechem.2025.04.043

Chengcai Liu , Yuanxing Zhang , Yawen Liu , Ling Zhang , Xuefeng Wang , Daobin Mu , Borong Wu

{"title":"Reasonable control of cut-off voltage to achieve stable lithium metal anode","authors":"Chengcai Liu , Yuanxing Zhang , Yawen Liu , Ling Zhang , Xuefeng Wang , Daobin Mu , Borong Wu","doi":"10.1016/j.jechem.2025.04.043","DOIUrl":"10.1016/j.jechem.2025.04.043","url":null,"abstract":"<div><div>Uneven lithium deposition leading to lithium dendrite growth severely hampers the application of lithium-metal batteries. Modifying the collector with lithiophilic materials helps improve lithium deposition. For lithophilic materials to modify the collector, the choice of cut-off voltage is very important. While excessively high cut-off voltages may compromise the stability of the modified layer and consequently disrupt ordered lithium deposition, conventional approaches typically employ lower cut-off voltages (particularly 0.1 V) to maintain modification layer stability. However, the 0.1 V cut-off voltage results in incomplete lithium stripping from the lithiophilic material surface. This phenomenon significantly diminishes the lithiophilic properties of the modified layer and consequently leads to substantial nucleation overpotential. Here, we propose to use a moderate cut-voltage stimulation effect to slow down the interfacial shielding effect of residual lithium metal on lithiophilic materials. By optimizing the cut-off voltage for the Cu@Sb<sub>2</sub>S<sub>3</sub> collector, the stability of the modified layer can be preserved while enabling the complete stripping of lithium metal from the surface of the lithophilic material. The asymmetric cell received the highest Coulombic efficiency (CE) when the lithium stripping cut-off voltage was set at 0.5 V relative to 0.1 and 2.0 V. At a current density of 1 mA cm<sup>−2</sup> and a deposition capacity of 1 mA h cm<sup>−2</sup>, the CE remained 98.6% at a cut-off voltage of 0.5 V after 140 cycles in an ether electrolyte without lithium nitrate.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 961-971"},"PeriodicalIF":13.1,"publicationDate":"2025-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114971","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

Suppression of light-induced phase segregation in all-inorganic wide-bandgap perovskite solar cells via molecular interaction design 分子相互作用设计抑制全无机宽禁带钙钛矿太阳能电池光致相偏析

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-27 DOI: 10.1016/j.jechem.2025.04.046

Jing Yang , Yunlong Gan , Mengqi Han , Shiheng Wang , Pengwei Li , Yiqiang Zhang , Gang Li , Yanlin Song

{"title":"Suppression of light-induced phase segregation in all-inorganic wide-bandgap perovskite solar cells via molecular interaction design","authors":"Jing Yang , Yunlong Gan , Mengqi Han , Shiheng Wang , Pengwei Li , Yiqiang Zhang , Gang Li , Yanlin Song","doi":"10.1016/j.jechem.2025.04.046","DOIUrl":"10.1016/j.jechem.2025.04.046","url":null,"abstract":"<div><div>Wide-bandgap mixed-halide perovskites, particularly CsPbIBr<sub>2</sub>, hold great promise for multi-junction solar cells due to their well-matched bandgap and all-inorganic material system. However, their inherent susceptibility to light-induced phase segregation (LIPS) limits efficiency and stability. In this work, we investigate the effect of three organic additives—4-cyclopentene-1,3-dione (CPD), maleimide (HPD), and 3,4-dibromo-1H-pyrrole-2,5(2H,5H)-dione (BrPD)—on LIPS in wide-bandgap CsPbIBr<sub>2</sub> perovskite films. The additives form various chemical interactions, including coordination bonds, hydrogen bonds, and ionic bonds, with I<sup>−</sup> and undercoordinated Pb<sup>2+</sup> ions, among which BrPD has the strongest interaction. This interaction regulates crystallization and improves film morphology. The BrPD-modified films have the largest grain size and the highest light stability, suppressing LIPS, enhancing carrier transfer, and improving device performance. BrPD-modified CsPbIBr<sub>2</sub>-based solar cells achieve a power conversion efficiency (PCE) of 11.34%, outperforming the control (8.96%) and other additives. Moreover, BrPD-modified devices show excellent stability, retaining 94% of their initial PCE after 60 min of continuous light exposure. This work highlights the potential of strategically selected organic additives to enhance the stability and performance of perovskite solar cells, offering valuable insights for the design of high-efficiency and long-lasting perovskite-based optoelectronic devices.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 550-557"},"PeriodicalIF":13.1,"publicationDate":"2025-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072591","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

Gallium-substituted self-pillared pentasil nanosheets combined with metal oxides for CO2 hydrogenation with enhanced selectivity of gasoline 镓取代自柱五戊二烯纳米片与金属氧化物结合用于二氧化碳加氢，提高汽油的选择性

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-27 DOI: 10.1016/j.jechem.2025.04.045

Fengli Yuan , Wenhui Li , Hong Yang , Guangjin Hou , Kuizhi Chen , Junhui Yu , Min Liu , Xinwen Guo

{"title":"Gallium-substituted self-pillared pentasil nanosheets combined with metal oxides for CO2 hydrogenation with enhanced selectivity of gasoline","authors":"Fengli Yuan , Wenhui Li , Hong Yang , Guangjin Hou , Kuizhi Chen , Junhui Yu , Min Liu , Xinwen Guo","doi":"10.1016/j.jechem.2025.04.045","DOIUrl":"10.1016/j.jechem.2025.04.045","url":null,"abstract":"<div><div>Carbon dioxide hydrogenation to gasoline can effectively alleviate the energy crisis and benefit the global environment. Owing to its orthogonally connected nanosheet configuration, large pore volume, and appropriate thickness of single nanosheet, self-pillared pentasil (SPP) nanosheet zeolite is integrated with In<sub>2</sub>O<sub>3</sub>-ZrO<sub>2</sub> as a tandem catalyst for CO<sub>2</sub> hydrogenation to C<sub>5+</sub> hydrocarbons. By substituting Al in the SPP framework with Ga, the acid strength of SPP is reduced, and acid density is increased, which favors the generation of C<sub>5+</sub> hydrocarbons and enhances the cracking resistance of long-chain hydrocarbons. A maximum C<sub>5+</sub> hydrocarbon selectivity of 82% was obtained on In<sub>2</sub>O<sub>3</sub>-ZrO<sub>2</sub>/Ga-SPP (Si/Ga = 100), which shows no deactivation after 200 h reaction time. Furthermore, introducing Pd into the In<sub>2</sub>O<sub>3</sub>-ZrO<sub>2</sub> not only boosts CO<sub>2</sub> conversion to 11% but also suppresses methane selectivity to below 1%. This study offers valuable insights into the design of highly active CO<sub>2</sub>-to-gasoline catalysts by leveraging the distinctive structure and acidity of zeolites within the tandem catalyst systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 517-526"},"PeriodicalIF":13.1,"publicationDate":"2025-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072588","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

Challenges and strategies for the cyclic stability of Ni-rich layered oxide cathode materials 富镍层状氧化物正极材料循环稳定性的挑战与对策

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-26 DOI: 10.1016/j.jechem.2025.04.039

Hongbing Ding , Yang Su , Xinlu Wang , Yue Hu , Xin Li , Hongbo Zhang , Guixia Liu , Wensheng Yu , Xiangting Dong , Jinxian Wang , Xin Wang

{"title":"Challenges and strategies for the cyclic stability of Ni-rich layered oxide cathode materials","authors":"Hongbing Ding , Yang Su , Xinlu Wang , Yue Hu , Xin Li , Hongbo Zhang , Guixia Liu , Wensheng Yu , Xiangting Dong , Jinxian Wang , Xin Wang","doi":"10.1016/j.jechem.2025.04.039","DOIUrl":"10.1016/j.jechem.2025.04.039","url":null,"abstract":"<div><div>Ni-rich cathode materials have become the mainstream choice in the mileage electric vehicle sector due to their high specific capacity and safety factor. However, the volume changes occurring during charging and discharging lead to microcracking and surface remodeling, posing challenges to achieving such as high specific capacity and long cycle stability. This paper reviews existing modification strategies for Ni-rich layered oxide cathode materials. Unlike previous reviews and related papers, we comprehensively discuss a variety of modification strategies and deeply discuss the synergistic modification effect of surface coating and bulk doping, which is how to improve the cycling stability of the Ni-rich cathode. In addition, based on recent research advances, the prospects and challenges of modifying Ni-rich layered cathodes for cycle stability upgrading of the lithium-ion battery, as well as the potential application prospects in the field of power automobiles, are comprehensively analyzed.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 427-457"},"PeriodicalIF":13.1,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071135","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

Dual-phase spinel manganese-cobalt hybrid oxide for enhanced oxygen evolution catalysis in acid media 双相尖晶石锰钴杂化氧化物在酸性介质中增强析氧催化

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-26 DOI: 10.1016/j.jechem.2025.04.042

Mengwei Guo , Ze Zhang , Hangrui Zhang , Jiajun Lin , Xianshu Qin , Rongrong Deng , Mingyuan Gao , Qibo Zhang

{"title":"Dual-phase spinel manganese-cobalt hybrid oxide for enhanced oxygen evolution catalysis in acid media","authors":"Mengwei Guo , Ze Zhang , Hangrui Zhang , Jiajun Lin , Xianshu Qin , Rongrong Deng , Mingyuan Gao , Qibo Zhang","doi":"10.1016/j.jechem.2025.04.042","DOIUrl":"10.1016/j.jechem.2025.04.042","url":null,"abstract":"<div><div>Developing efficient and durable non-noble-metal catalysts for the oxygen evolution reaction (OER) in acidic media remains a critical challenge for proton-exchange membrane water electrolysis. Here, we report a dual-phase Mn<sub>3</sub>O<sub>4</sub>-Co<sub>2</sub>MnO<sub>4</sub> hybrid oxide electrocatalyst synthesized via a sulfur-assisted co-electrodeposition strategy in a choline chloride/ethylene glycol-based deep eutectic solvent, followed by annealing. The incorporation of sulfur facilitates the formation of a cubic spinel Co<sub>2</sub>MnO<sub>4</sub> phase within the Mn<sub>3</sub>O<sub>4</sub> host, optimizing electronic conductivity and stabilizing the catalytic layer by strengthening Mn–O bonds. When supported on a corrosion-resistant Pt/Ti substrate, the composite electrode achieves a low overpotential of 317 mV at 10 mA cm<sup>−2</sup> and sustains stable operation for over 100 h in 0.05 M H<sub>2</sub>SO<sub>4</sub> (pH = 1), outperforming most MnO<em><sub>x</sub></em>-based catalysts and approaching noble-metal benchmarks. Density functional theory calculations reveal that the Co<sub>2</sub>MnO<sub>4</sub> phase lowers the energy barrier for the rate-determining OOH* → O<sub>2</sub> step, while in-situ spectroscopic analyses confirm its structural integrity under acidic OER conditions. Furthermore, electrolyte dissociation kinetics significantly influences performance, with HClO<sub>4</sub> exhibiting superior mass transfer due to its high proton conductivity. This work provides a rational design pathway for non-noble-metal acidic OER catalysts through phase engineering and electrolyte optimization, advancing sustainable hydrogen production technologies.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 361-372"},"PeriodicalIF":13.1,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068007","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

Construction of efficient electrodes for CO2RR through microenvironment regulation of hydrophobic ionomer 疏水离聚体微环境调控构建高效CO2RR电极

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-26 DOI: 10.1016/j.jechem.2025.04.040

Qingfeng Chang , Gong Zhang , Jinxing Chen , Xiaowei Du , Chujun Wang , Yuan Cai , Yuzhe Du , Peng Zhang , Tuo Wang , Jinlong Gong

{"title":"Construction of efficient electrodes for CO2RR through microenvironment regulation of hydrophobic ionomer","authors":"Qingfeng Chang , Gong Zhang , Jinxing Chen , Xiaowei Du , Chujun Wang , Yuan Cai , Yuzhe Du , Peng Zhang , Tuo Wang , Jinlong Gong","doi":"10.1016/j.jechem.2025.04.040","DOIUrl":"10.1016/j.jechem.2025.04.040","url":null,"abstract":"<div><div>CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) electrolyzers based on gas diffusion electrode (GDE) enable the direct mass transfer of CO<sub>2</sub> to the catalyst surface for participation in the reaction, thereby establishing an efficient three-phase reaction interface that significantly enhances current density. However, current hydrophobic modification methods face difficulties in achieving precise and substantial control over wettability, and the hydrophobic modifiers tend to significantly impair the conductivity of the electrode and ion transport capabilities. This study employs Nafion ionomers to hydrophobically modify the three-dimensional catalyst layer, revealing the bifunctionality of Nafion. The fluorinated backbone of Nafion ensures the hydrophobicity of the entire catalyst layer, while its sulfonic acid groups promote ion transport, without significantly affecting the conductivity of the electrode. Furthermore, by employing modifiers with distinct wettability characteristics, a highly efficient and large-scale manipulation of the hydrophilic/hydrophobic properties of the catalyst layer was successfully realized. The electrode, constructed with silver nanopowder as a representative catalyst and modified with the hydrophobic ionomer Nafion, exhibits a substantial enhancement in both catalytic activity and durability. The optimized electrode exhibited exceptional electrocatalytic performance in both flow cell and membrane electrode assembly (MEA) configurations. Notably, in the MEA, the electrode achieved a remarkable CO Faradaic efficiency (FE) of 93.3% at a total current density of 200 mA cm<sup>−2</sup>, while maintaining stable operation for over 62 h.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 373-380"},"PeriodicalIF":13.1,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071899","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

Sintering- and water-resistant perovskite quantum dots supported by inorganic materials for enhanced luminescence 无机材料支持的增强发光的烧结和防水钙钛矿量子点

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-26 DOI: 10.1016/j.jechem.2025.04.041

Meng Wu , Lingxiang Sun , Yanjie Zhang , Feng Hong , Xunzhu Jiang , Xiuping Wu , Chunwen Ye , Jingjie Yu , Bing Li , Botao Qiao

{"title":"Sintering- and water-resistant perovskite quantum dots supported by inorganic materials for enhanced luminescence","authors":"Meng Wu , Lingxiang Sun , Yanjie Zhang , Feng Hong , Xunzhu Jiang , Xiuping Wu , Chunwen Ye , Jingjie Yu , Bing Li , Botao Qiao","doi":"10.1016/j.jechem.2025.04.041","DOIUrl":"10.1016/j.jechem.2025.04.041","url":null,"abstract":"<div><div>Metal halide perovskite quantum dots (MHPQDs) have attracted intensive interest because of their unique optoelectronic properties. Their undesirable degradation upon exposure to humidity and/or heat, however, poses a dear challenge for the practical applications. Herein we report a facile strategy to develop sintering-resistant MHPQDs, e.g. CsPbBr<sub>3</sub>, by localizing them on the surface of inorganic support such as hydroxyapatite (HAP). The chemical interaction between CsPbBr<sub>3</sub> quantum dots (QDs) and HAP support originates from the occupation of Br vacancies in CsPbBr<sub>3</sub> by the –O<sup>−</sup> on the surface of HAP support, which not only stabilizes the small particle sizes (∼2.2 nm) of CsPbBr<sub>3</sub> QDs upon high-temperature (up to 400 °C) calcination but also greatly enhances its photoluminescence emission intensity by about 150 times. Interestingly, the supported CsPbBr<sub>3</sub> QDs decorated by cetyltrimethylammonium bromide can further produce water-resistant CsPbBr<sub>3</sub>@CsPb<sub>2</sub>Br<sub>5</sub> QDs. The obtained sintering-resistant hydroxyapatite-supported CsPbBr<sub>3</sub>@CsPb<sub>2</sub>Br<sub>5</sub> QDs can be used to fabricate green light emitting diodes (LED) devices with high luminous intensity for medicolegal identification, flexible luminescence film for display, and potential fluorescent label for bioimaging/biosensing applications. This work demonstrates a novel strategy to design and develop robust all-inorganic QDs composites that may find wide applications in diverse environmental conditions, including high temperature and/or high humidity.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 508-516"},"PeriodicalIF":13.1,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072589","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

Three-dimensional covalent organic framework photocatalyst with asymmetrically coordinated single-atom cobalt for highly efficient CO2 reduction reactions 具有不对称配位单原子钴的三维共价有机框架光催化剂用于高效的CO2还原反应

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-25 DOI: 10.1016/j.jechem.2025.04.032

Wuqing Luo , Jia Chen , Zhuozhuo Tang , Baopeng Yang , Guoxin Chen , Shengyao Wang , Gen Chen , Min Liu , Hong Xu , Jinhua Ye , Ning Zhang

{"title":"Three-dimensional covalent organic framework photocatalyst with asymmetrically coordinated single-atom cobalt for highly efficient CO2 reduction reactions","authors":"Wuqing Luo , Jia Chen , Zhuozhuo Tang , Baopeng Yang , Guoxin Chen , Shengyao Wang , Gen Chen , Min Liu , Hong Xu , Jinhua Ye , Ning Zhang","doi":"10.1016/j.jechem.2025.04.032","DOIUrl":"10.1016/j.jechem.2025.04.032","url":null,"abstract":"<div><div>Three-dimensional (3D) covalent organic frameworks (COFs) have attracted extensive attention as photocatalysts for CO<sub>2</sub> reduction reactions. Introducing metal atoms is essential for enhancing activity, but previous metal sites in 3D COFs predominantly exhibit symmetrical coordination, making them unsuitable for CO<sub>2</sub> activation. Here, we design a 3D COF with 2,2′-pyridine linked around tetra-(4-anilyl)methane (TCM-Bpy-COF), where Co<sup>2+</sup> is asymmetrically coordinated by bipyridine and acetates (TCM-Bpy-COF-CoAc). The TCM-Bpy-COF-CoAc exhibits outstanding photocatalytic CO<sub>2</sub> reduction performance under weak visible light, achieving a CO evolution rate of 26,650 μmol g<sup>−1</sup> h<sup>−1</sup> under 5 W of light-emitting-diode (LED) lamp and high apparent quantum efficiency. The performance far exceeds that of symmetrically coordinated bipyridine-Co-bipyridine TCM-Bpy-COF and surpasses most reported COF-based photocatalysts. In-situ spectral characterizations and theoretical calculations show that asymmetric N, O-coordination around the Co<sup>2+</sup> center polarizes electron density and lowers reaction energy barriers of *COOH intermediates, enhancing the conversion of CO<sub>2</sub> to CO. This work inspires the design of 3D COF-based photocatalysts with highly catalytic efficiency.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 400-409"},"PeriodicalIF":13.1,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071204","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

Switching the product selectivity from methane to methanol in CO2 hydrogenation via Cu-modified vacancy engineering at MoS2 edge sites

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-04-25 DOI: 10.1016/j.jechem.2025.04.038

Guanghui Zhang , Xin Meng , Hao Wang , Zhiqun Wang , Hui Gao , Mingrui Wang , Chunshan Song , Xinwen Guo

{"title":"Switching the product selectivity from methane to methanol in CO2 hydrogenation via Cu-modified vacancy engineering at MoS2 edge sites","authors":"Guanghui Zhang , Xin Meng , Hao Wang , Zhiqun Wang , Hui Gao , Mingrui Wang , Chunshan Song , Xinwen Guo","doi":"10.1016/j.jechem.2025.04.038","DOIUrl":"10.1016/j.jechem.2025.04.038","url":null,"abstract":"<div><div>The catalytic hydrogenation of carbon dioxide (CO<sub>2</sub>) to methanol (CH<sub>3</sub>OH) represents a promising strategy for mitigating carbon emissions and closing the carbon cycle. This study demonstrates that the incorporation of Cu into MoS<sub>2</sub> catalysts significantly enhances methanol selectivity and productivity. Through a combination of transmission electron microscope, X-ray diffraction, Raman, electron paramagnetic resonance, X-ray photoelectron spectroscopy, diffuse reflectance Infrared Fourier transform spectroscopy, X-ray absorption spectroscopy, temperature-programmed desorption, and kinetic analysis, we reveal that Cu modifies edge sulfur vacancies, thereby suppressing methane formation and promoting methanol synthesis. At 220 °C and 5 MPa, the 2%Cu/MoS<sub>2</sub> catalyst achieves 85.5% selectivity toward CH<sub>3</sub>OH, and the methanol formation rate reaches 7.88 mmol g<sup>−</sup><sup>1</sup><sub>cat</sub> h<sup>−1</sup> (0.256 mmol <span><math><mrow><msubsup><mrow><mi>m</mi></mrow><mrow><msub><mrow></mrow><mrow><msub><mrow><mi>MoS</mi></mrow><mrow><mn>2</mn></mrow></msub></mrow></msub></mrow><mrow><mo>-</mo><mn>2</mn></mrow></msubsup></mrow></math></span> h<sup>−1</sup>), representing the highest performance among MoS<sub>2</sub>-based catalysts under comparable conditions. This work provides an efficient and potentially scalable approach for designing advanced MoS<sub>2</sub>-based catalysts for CO<sub>2</sub> hydrogenation.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 286-296"},"PeriodicalIF":13.1,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143943292","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