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Versatile Inorganic Oligomer-based Photochromic Spiropyrane Gels
Jiajia Song, Wei Duan, Yun Chen* and Xiangyang Liu*
Versatile Inorganic Oligomer-based Photochromic Spiropyrane Gels
Jiajia Song, Wei Duan, Yun Chen* and Xiangyang Liu*
In this cover picture, a green inorganic oligomer-based spiropyrans composite gelatinous system is constructed based on the calcium ionic nanocrystalline core controlled by capping agent TEA and the flexible cavities in soft materials surrounding the nanocrystalline. This material exhibits excellent cyclic reversible discoloration properties and application potential for hydrazine detection.
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ReviewConductive Metal/Covalent Organic Frameworks for CO2 ElectroreductionChang-Pu Wan, Jun-Dong Yi, Rong Cao* and Yuan-Biao Huang*
Chin. J. Struct. Chem. 2022, 41, 2205001-2205014 DOI: 10.14102/j.cnki.0254-5861.2022-0075
May 20, 2022
metal-organic frameworks, covalent organic frameworks, CO2 electroreduction reaction, conductive frameworks
ABSTRACT
Porous crystalline metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) are promising platforms for electrocatalytic reduction of CO2(CO2RR) due to their large CO2 adsorption uptakes and periodically arranged single active sites. However, the applications in CO2RR of the traditional MOFs and COFs are greatly limited by their low electron conductivity. In recent years, numerous types of MOFs and COFs with high intrinsic conductivity have been rationally designed and successfully constructed, and some of them have been applied in CO2RR. In this review, the applications of conductive MOFs and COFs in CO2RR have been summarized. The conductive MOFs and COFs can be categorized according to the methods, in which the conductivity is enhanced, such as constructing fully π-conjugated backbones, donor-acceptor heterojunction, enhancing the π-π stacking interactions between organic moieties and/or the introduction of guest molecules. -
ReviewSolar-Powered Environmentally Friendly Hydrogen Production: Advanced Technologies for Sunlight-Electricity-Hydrogen NexusWeiquan Ji, Kang Zhang, Ke Zhan, Ping Wang, Xianying Wang* and Ya Yan*
Chin. J. Struct. Chem. 2022, 41, 2205015-2205029 DOI: 10.14102/j.cnki.0254-5861.2022-0106
May 20, 2022
water splitting, hydrogen production, green coupling system, sunlight-electricity-hydrogen, structure-activity relations
ABSTRACT
Hydrogen production from water splitting is a clean and sustainable hydrogen production route to alleviate the current energy crisis. However, factors such as energy conversion efficiency, cost-effectiveness, and social benefit limit their industrial application. Therefore, the develop- ment of advanced water splitting technologies using clean and renewable energy has become an important research goal of the world. Converting endless solar energy into hydrogen energy directly or indirectly is an effective way to reduce the energy input of hydrogen production. This review focuses on the latest advances in the coupling design of renewable energy supply devices and catalytic electrodes in hydrogen production systems. We not only review the single hydrogen production system based on photochemical, photoelectrochemical, photovoltaic, thermoelectric, pyroelectric, and piezoelectric devices, but also discuss the complex systems of the multiple devices. The structural design of energy supply devices and catalytic electrodes and the study of hydrogen production performance in different systems will be critically discussed in this work. Finally, current challenges and future perspectives of advanced technologies for sunlight-electricity-hydrogen nexus are also presented. It is hoped that this review will provide a timely reference for advancing the development of sunlight-electricity-hydrogen nexus and thus achieve the goal of sustainable production of green hydrogen. -
ArticleBoosting Stable and Fast Potassium Storage of Iron Sulfide through Rational Yolk-Shell Design and Ni Doping
Yanmei Gan, Jiajie Zhu, Qixin Zhang, Chaoying Wang, Lunhui Guan and Yi Zhao*
Chin. J. Struct. Chem. 2022, 41, 2205030-2205036 DOI: 10.14102/j.cnki.0254-5861.2022-0044
May 20, 2022
FeS2, Ni-doping, yolk-shell structure, anode, potassium-ion batteries
ABSTRACT
Metal sulfides have been regarded as promising anodes for potassium-ion batteries (PIBs) due to their high theoretical capacities, while the performance is limited by their intrinsic poor conductivity and large volume fluctuation during the insertion/extraction of large potassium ion. Herein, the battery performance of iron sulfide anode is significantly enhanced through yolk-shell (Y-S) structure design and nickel doping, aiming to realize good structure stability and superior electron/ion transportation. For potassium storage, as-prepared Y-S Ni-FeS2@C shows excellent cyclic performance and sustains high capacities of 328 mA h g-1 after 100 cycles at 0.2 A g-1 and 226 mA h g-1 after 1000 cycles at 1 A g-1. Especially, it displays a superior rate capacity of 200 mA h g-1 at 20 A g-1, higher than that of Y-S FeS2@C and most as-reported metal sulfide anodes for PIBs. The experimental analysis and theoretical calculation illuminate the effect of Ni-doping on decreasing the particle size of iron sulfide and enhancing the ion/electron transport ability, thus accounting for the exceptional rate capability of Y-S Ni-FeS2@C composite. -
ArticleVersatile Inorganic Oligomer-Based Photochromic Spiropyrane GelsJiajia Song, Wei Duan, Yun Chen* and Xiangyang Liu*
Chin. J. Struct. Chem. 2022, 41, 2205037-2205047 DOI: 10.14102/j.cnki.0254-5861.2022-0061
May 20, 2022
inorganic oligomer, photochromic, gels, naked-eye detection of hydrazine
ABSTRACT
Here we report an example of a general strategy for the immobilization of various different photochromic spiropyran molecules on eco-friendly cheap nanomatrix. The spiropyrans are encapsulated in calcium salt oligomers-based gels by centrifugation, forming an inorganic oligomer-based gelatinous photoswitchable hybrid material. Ca2+ is also used to regulate the optical properties of spiropyrans through chelation. The oligomer-based gel can not only provide the space required for photoisomerization, but also reduce the interference of the surrounding environment on the photochromic properties. Moreover, a practical paper-based and colloidal flexible substrate platform is constructed for the removal and naked-eye detection of liquid and gaseous hydrazine at room temperature based on the reactivity of the formyl group on spiropyrans loaded in Ca3(PO4)2 oligomers. This general strategy can be used for other inorganic oligomer-based molecular switches and sensing systems. -
ArticlePolymeric Wetting Matrix for a Stable Interface between Solid-State Electrolytes and Li Metal AnodeHaoran Song, Shida Xue, Shiming Chen, Zijian Wang, Yongli Song, Jiawen Li, Zhibo Song, Luyi Yang* and Feng Pan*
Chin. J. Struct. Chem. 2022, 41, 2205048-2205054 DOI: 10.14102/j.cnki.0254-5861.2022-0067
May 20, 2022
Li metal, Li dendrite, poly(methyl methacrylate), succinonitrile, composite solid-state electrolyte
ABSTRACT
Succinonitrile (SN) based solid-state electrolytes (SSEs) have potential applications in lithium (Li) batteries due to their ease of preparation and high ionic conductivity at room temperature. Here, a novel SSE consisting of poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP), poly(methyl methacrylate) (PMMA) and Li1.3Al0.3Ti1.7(PO4)3 with SN is fabricated, where PMMA is added to serve as a polymer matrix for better wettability of SN. Due to the addition of PMMA, improved room-temperature ionic conductivity of the SSE is resulted. More importantly, better interfacial contact as well as more stable solid electrolyte interphase (SEI) layer between SSE and Li anode can be also obtained. As a result, homo- geneous and dendrite-free Li plating can be achieved for over 1000 h in Li symmetric cells. When coupled with LiNi0.5Mn0.3Co0.2O2 cathode and Li anode, the proposed SSE delivers excellent cycling stability and rate capability in full-cells. By implementing SSEs with a polymeric wetting agent, this work provides fresh perspectives on stabilizing the interface between SSEs and Li metal anodes. -
ArticleAn Advanced Design Concept of Mansion-Like Freestanding Silicon Anodes with Improved Lithium Storage PerformancesDeqing Zhang, Junfeng Ren, Caixia Li*, Bin Luo*, Lei Wang* and Yanyan Li
Chin. J. Struct. Chem. 2022, 41, 2205055-2205062 DOI: 10.14102/j.cnki.0254-5861.2022-0070
May 20, 2022
Si anode, bacterial cellulose, graphene, 3D conductive network, binder-free, lithium-ion battery
ABSTRACT
To conquer inherently low conductivity, volume swelling, and labile solid electrolyte interphase (SEI) films of Si anode in lithium ion battery (LIBs), it is widely accepted that appropriate structure design of Si-C hybrids performs effectively, especially for nanosize Si particles. Herein, inspired by the sturdy construction of high-rise buildings, a mansion-like 3D structured Si@SiO2/PBC/RGO (SSPBG) with separated rooms is developed based on 0D core-shell Si@SiO2, 1D pyrolytic bacterial cellulose (PBC) and 2D reduced graphene oxide (RGO). Therefore, these hierarchical protectors operate synergistically to inhibit the inevitable volume changes during electrochemical process. Specifically, tightly coated SiO2shell as the first protective layer could buffer the volume expansion and reduce detrimental pulverization of Si NPs. Furthermore, flexible spring-like PBC and ultra-fine RGO sheets perform as securer barriers and skeleton which will counteract the microstructure strain and accelerate electron transfer at the same time. Remarkably, the self-supporting electrode realizes a distinguished performance of 901 mAh g-1at 2 A g-1 for 500 cycles. When matched with LiFePO4 cathodes, high stability of more than 100 cycles has been realized for the full batteries. -
ArticleSelective Electrocatalytic Hydrogenation of 5-Hydroxymethyl-furfural to 2,5-Dihydroxymethylfuran on Bimetallic PdCu Alloy
Xu Yue, Weixing Zhao, Shuangyin Wang and Yuqin Zou*
Chin. J. Struct. Chem. 2022, 41, 2205063-2205069 DOI: 10.14102/j.cnki.0254-5861.2022-0074
May 20, 2022
biomass, 2,5-dihydroxymethylfuran, electrocatalyst, bimetallic alloy, hydrogenation
ABSTRACT
2,5-Dihydroxymethylfuran (DHMF), obtained from 5-hydroxymethylfurfural (HMF) by electrochemical method, is a promising building block for polymers. However, one challenge of this process is to reduce initial potential and improve catalytic selectivity. In this work, the PdCu bimetallic catalyst is prepared with an onset potential of -0.05 VRHE and a selectivity of 99%. Compared with the single Cu electrocatalyst, the adsorption of HMF and proton is improved by introducing of Pd, which is demonstrated by the electrochemical results and hydrogen production rate. This work provides an effective strategy to improve the selectivity of Cu-based electrocatalyst and builds a relationship between the adsorption capacity and the electrocatalytic performance. -
Morphology Engineering toward Highly Emissive Mn2+ Doped PEA2PbBr4 Perovskite with Their LED Application via Phosphonium PassivationYu-Feng Sang, Liang-Jin Xu* and Zhong-Ning Chen*
Chin. J. Struct. Chem. 2022, 41, 2205070-2205076 DOI: 10.14102/j.cnki.0254-5861.2022-0088
May 20, 2022
2D perovskite, Mn2+ doped, energy transfer, perovskite LED
ABSTRACT
Mn2+-doped lead halide perovskites either in 3D or 2D have been extensively explored due to their rich energy-transfer behaviors. While their application on LED is still lagging behind in comparison to non-doped 3D perovskite due to inferior film-formation and low luminescent efficiency. Here we report an in-situ-formed Mn2+ doped 2D perovskite nanocrystal (NCs) film by introducing quaternary phosphonium salt during the crystallizing process. The as-formed film shows improved luminescent efficiency with emission peaked at 600 nm and photoluminescence quantum yield (PLQY) of as high as 73.37%, which is about 1.3 times higher than that of pristine film. Further characterizations confirm the enhanced confinement effect from smaller size particle is responsible for the improved luminescent efficiency. The perovskite LEDs based on pristine and phosphonium passivated thin films were fabricated, and a great improvement in the external quantum efficiency of these LEDs (from 0.0017% to 0.12%) is observed due to the improved morphology and enhanced luminescent efficiency. -
ArticleContributions of Cs and Rb on Inhibiting Photo-induced Phase Segregation and Enhancement Optoelectronic Performances of MA1-yXyPbI1.8Br1.2(X = Cs, Rb) Single Crystals
Qing Yao, Kaiyu Wang, Jie Zhang, Changqian Li, Chenyu Shang, Feitong Chen, Qi Huang, Qiqi Zhao, Weiwei Zhang, Xiaoyuan Zhan and Jianxu Ding*
Chin. J. Struct. Chem. 2022, 41, 2205077-2205084 DOI: 10.14102/j.cnki.0254-5861.2022-0089
May 20, 2022
perovskite single crystal, photo-induced phase segregation, mixed A-cation, optoelectronic performances
ABSTRACT
Introducing inorganic cation into hybrid organic-inorganic perovskites (HOIPs) has attracted great attention because of the enhancement stabilities without sacrificing their excellent optoelectronic properties. Here, we introduce Cs and Rb into MAPbI1.8Br1.2 single crystals (SCs) to dig out the mixed cation effect on optoelectronic performances and phase stabilities. Both Rb and Cs can increase the lattice capacity, which is sufficient to relieve the lattice stress caused by photon energy, thus achieving the purpose of stabilizing the lattice structure and inhibiting migration of halide ions, compared with MAPbI1.8Br1.2 SC. On the other hand, the smaller polarity of Rb and Cs reduces the electron-phonon coupling, thus significantly inhibiting the migration of halide ions. Meanwhile, through planar photo-detectors, MA0.9Cs0.1PbI1.8Br1.2-based device behaves much excellent optoelectronic performance (R = 0.170 A/W, EQE = 51.39 %, D*= 4.42 × 1012Jones, on/off ratio: ~522). -
ArticleZnMn3O7: A New Layered Cathode Material for Fast-Charging Zinc-Ion BatteriesRuitao Sun, Qin Liu and Wenzhuo Deng*
Chin. J. Struct. Chem. 2022, 41, 2205085-2205092 DOI: 10.14102/j.cnki.0254-5861.2022-0092
May 20, 2022
layered structure, zinc-manganese oxide, cathode, zinc-ion battery
ABSTRACT
Low-cost and high-energy-density manganese-based compounds are promising cathode materials for rechargeable aqueous zinc-ion batteries (AZIBs), however, they often experience cycling instability issues and inferior rate capability. Herein, we report a new layered manganese-based cathode material, ZnMn3O7 (ZMO), which possesses a large interlayer spacing of 4.8 Å and allows the intercalation of ~1.23 Zn-ions per formula unit (corresponding to a capacity of ~170 mAh/g). Importantly, ZMO exhibits good cycling stability (72.9% capacity retention over 400 cycles), ultrafast-charging capability (73% state of charge in 1.5 min), and an ultrahigh power density (3510 W/kg at 88 Wh/kg). Through kinetic characterization, the favorable diffusion of ions and the dominant capacitor contribution are found to be conducive to the achievement of superior fast charging capability. Furthermore, the charge storage mechanism is revealed by ex-situ XRD and ex-situ XPS. This work may shed light on the design of high-performance electrode materials for AZIBs. -
Highly Efficient Quasi-Homogeneous System for Photocatalytic H2O2 ProductionHuinan Che and Yanhui Ao*
Chin. J. Struct. Chem. 2022, 41, 2205093-2205094. DOI: 10.14102/j.cnki.0254-5861.2022-0107
May 20, 2022
ABSTRACT
The quasi-homogeneous photocatalytic system can be formed by iodide ions induced fragmented and ultrathin structured TP-PCN. The TP-PCN possesses abundant edge active sites, which can greatly enhance the O2 adsorption/ activation capacity and the 2e- ORR selectivity. As expected, the quasi-homogeneous system affords a remarkably increased photocatalytic H2O2 production activity.
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