IF 5.9 4区化学

结构化学 Pub Date : 2024-07-01 DOI: 10.1016/j.cjsc.2024.100290

{"title":"Cycad-leaf-like crystalline-amorphous heterostructures for efficient urea oxidation-assisted water splitting","authors":"","doi":"10.1016/j.cjsc.2024.100290","DOIUrl":"10.1016/j.cjsc.2024.100290","url":null,"abstract":"<div>Developing efficient bifunctional catalysts for urea oxidation reaction (UOR)/hydrogen evolution reaction (HER) is important for energy-saving hydrogen production. Herein, a catalyst with crystalline-amorphous heterostructure supported by NiCo alloy on nickel foam (NiCoO-MoOx/NC) is reported for the first time. Through simple molybdenum salt etching, 2D NiCo alloy nanosheets are transformed into a unique 3D cycad-leaf-like structure with a super-hydrophilic surface. Simultaneously, the synergistic effect between crystalline NiCoO and amorphous MoOx improves the UOR and HER activity, merely requiring 1.28 V and −45 mV potentials to reach ±10 mA cm−2, respectively. Particularly, the UOR kinetics of NiCoO-MoOx/NC is enhanced significantly compared to that of NiCoO/NC. The electronic structure of NiCoO is modified by MoOx, enabling the rapid generation of NiOOH and CoOOH active species, which would accelerate the synergistic electrocatalytic oxidation of urea molecules. This work inspires the design of highly active and stable bifunctional catalysts for urea assisted H2 production.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 7","pages":"Article 100290"},"PeriodicalIF":5.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140603104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Mn-modulated Co–N–C oxygen electrocatalysts for robust and temperature-adaptative zinc-air batteries 用于坚固耐用且温度适应性强的锌-空气电池的锰调制 Co-N-C 氧电催化剂

IF 5.9 4区化学

结构化学 Pub Date : 2024-07-01 DOI: 10.1016/j.cjsc.2024.100302

{"title":"Mn-modulated Co–N–C oxygen electrocatalysts for robust and temperature-adaptative zinc-air batteries","authors":"","doi":"10.1016/j.cjsc.2024.100302","DOIUrl":"10.1016/j.cjsc.2024.100302","url":null,"abstract":"<div>Flexible zinc-air batteries (FZABs) are featured with safety and high theoretical capacity and become one of the ideal energy supply devices for flexible electronics. However, the lack of cost-effective electrocatalysts remains a major obstacle to their commercialization. Herein, we synthesized a porous dodecahedral nitrogen-doped carbon (NC) material with Co and Mn bimetallic co-embedding (CoxMn1−x@NC) as a highly efficient oxygen reduction reaction (ORR) catalyst for ZABs. The incorporation of Mn effectively modulates the electronic structure of Co sites, which may lead to optimized energetics with oxygen-containing intermediates thereby significantly enhancing catalytic performance. Notably, the optimized Co4Mn1@NC catalyst exhibits superior E1/2 (0.86 V) and jL (limiting current density, 5.96 mA cm−2) compared to Pt/C and other recent reports. Moreover, aqueous ZAB using Co4Mn1@NC as a cathodic catalyst demonstrates a high peak power density of 163.9 mW cm−2 and maintains stable charging and discharging for over 650 h. Furthermore, FZAB based on Co4Mn1@NC can steadily operate within the temperature range of −10 to 40 °C, demonstrating the potential for practical applications in complex climatic conditions.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 7","pages":"Article 100302"},"PeriodicalIF":5.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140609573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

2D zirconium-based metal-organic framework/bismuth(III) oxide nanorods composite for electrocatalytic CO2-to-formate reduction 二维锆基金属有机框架/氧化铋(III)纳米棒复合材料用于电催化二氧化碳到甲酸盐的还原反应

IF 5.9 4区化学

结构化学 Pub Date : 2024-07-01 DOI: 10.1016/j.cjsc.2024.100301

{"title":"2D zirconium-based metal-organic framework/bismuth(III) oxide nanorods composite for electrocatalytic CO2-to-formate reduction","authors":"","doi":"10.1016/j.cjsc.2024.100301","DOIUrl":"10.1016/j.cjsc.2024.100301","url":null,"abstract":"<div>Electrocatalytic carbon dioxide reduction reaction (eCO2RR) represents one of the most promising technologies for sustainable conversion of CO2 to value-added products. Although metal-organic frameworks (MOFs) can be vastly functionalized to create active sites for CO2RR, low intrinsic electrical conductivity always makes MOFs unfavorable candidates for eCO2RR. Besides, studies on how to regulate eCO2RR activity of MOFs from linkers' functionalities viewpoint lag far behind when compared with the assembly of multinuclear metal-centered clusters. In this work, non-toxic bismuth(III) oxide (Bi2O3) was incorporated into a series of two-dimensional (2D) MOFs (ZrLX) established from Zr-oxo clusters and triazine-centered 3-c linkers with different functionalities (LX = 1–5) to give composites ZrLX/Bi2O3. To investigate how functionalities on linkers distantly tune the eCO2RR performance of MOFs, electron-donating/withdrawing groups were installed at triazine core or benzoate terminals. It is found that ZrL2/Bi2O3 (‒F functionalized on triazine core) exhibits the best eCO2RR performance with the highest Faradaic efficiency (FE) of 96.73% at −1.07 V vs. RHE, the largest electroactive surface (Cdl = 4.23 mF cm−2) and the highest electrical conductivity (5.54 × 10−7 S cm−1), highlighting tuning linker functionalities and hence electronic structure as an alternative way to regulate eCO2RR.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 7","pages":"Article 100301"},"PeriodicalIF":5.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140593449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tandem catalysis for photoreduction of CO2 into multi-carbon fuels on atomically thin dual-metal phosphochalcogenides 在原子级双金属磷钙钛矿薄膜上串联催化二氧化碳光还原成多碳燃料

IF 5.9 4区化学

结构化学 Pub Date : 2024-07-01 DOI: 10.1016/j.cjsc.2024.100320

引用次数: 0

Design of two-dimensional porous covalent organic framework semiconductors for visible-light-driven overall water splitting: A theoretical perspective 设计用于可见光驱动整体水分离的二维多孔共价有机框架半导体：理论视角

IF 5.9 4区化学

结构化学 Pub Date : 2024-06-25 DOI: 10.1016/j.cjsc.2024.100375

{"title":"Design of two-dimensional porous covalent organic framework semiconductors for visible-light-driven overall water splitting: A theoretical perspective","authors":"","doi":"10.1016/j.cjsc.2024.100375","DOIUrl":"10.1016/j.cjsc.2024.100375","url":null,"abstract":"<div><div>Utilizing sunlight to split water into H2 and O2 is a highly promising approach in renewable energy production approaches. Recently, significant efforts have been devoted to developing innovative photocatalysts for splitting water. Metal-free two-dimensional (2D) covalent organic frameworks (COFs) are emerging as ideal catalytic platforms for this purpose. However, the rational design of these materials requires appropriate band alignment and active sites capable of catalyzing both hydrogen and oxygen evolution reactions (OERs), which depends on the judicious selection of molecular precursors. To address these requirements, first-principles calculations have proven to be an efficient method for designing and screening potential photocatalysts. Here, we provide a concise overview of recent advancements in the development of 2D COFs photocatalysts for overall water splitting (OWS), examining it from a theoretical perspective. This includes outlining the design principles, exploring the data-driven discovery of potential candidates using a COFs database, and applying machine learning (ML) techniques to predict the electronic structure of COFs based on the molecular orbitals of their precursors. Furthermore, we discuss the accuracy of current computational methods and address future challenges and potential of 2D COFs in practical applications for OWS.</div><div>© 2017 Elsevier Inc. All rights reserved.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 11","pages":"Article 100375"},"PeriodicalIF":5.9,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141512245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Rigid-flexible-ligand-ornamented lanthanide-incorporated selenotungstates and photoluminescence properties 刚性柔性配体饰有镧系元素的硒钨酸盐和光致发光特性

IF 5.9 4区化学

结构化学 Pub Date : 2024-06-22 DOI: 10.1016/j.cjsc.2024.100370

引用次数: 0

Structure and assembly mechanism of high-nuclear lanthanide-oxo clusters 高核镧系氧化物团簇的结构和组装机制

IF 5.9 4区化学

结构化学 Pub Date : 2024-06-19 DOI: 10.1016/j.cjsc.2024.100372

引用次数: 0

Atomically precise superatomic silver nanoclusters stabilized by O-donor ligands 由 O-供体配体稳定的原子精度超原子银纳米团簇

IF 5.9 4区化学

结构化学 Pub Date : 2024-06-19 DOI: 10.1016/j.cjsc.2024.100371