Chemical Research in Chinese Universities

Chemical Research in Chinese Universities Vol.39 No.1 February 2023

2023, 39(1): 1-4.

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This special issue provides a snapshot of the recent efforts on bio-inspired materials, including their unique properties, correlation between multiscale structures and properties, design and synthesis, and applications. We expect this issue can arouse more interest of readers in bio-inspired material chemistry, and then boost the progress of the related studies.

Self-assembled Supramolecular Artificial Transmembrane Ion Channels: Recent Progress and Application

LUO Yichen, ZHU Canhong, ZHANG Tianlong, YAN Tengfei, LIU Junqiu

2023, 39(1): 3-12. doi:10.1007/s40242-023-2337-5

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Natural protein channels have evolved with fantastic spatial structures, which play pivotal physiological functions in all living systems. Learning from nature, chemical scientists have developed a myriad of artificial transmembrane ion channels by using various chemical strategies, among which the non-covalent supramolecular ion channels exhibit remarkable advantages over other forms(e.g., single-molecule ion channel), which exhibited facile preparation methods, easier structural modification and functionalization. In this review, we have systematically summarized the recent progress of supramolecular self-assembled artificial transmembrane ion channels, which were classified by different self-assembly mechanisms, such as hydrogen bonds, π-π interactions, etc. Detailed preparation process and self-assembly strategies of the supramolecular ion channels have been described. Moreover, potential biomedical applications of the supramolecular ion channels have also been carefully discussed in this review. Finally, future opportunities and challenges facing this field were also elaborately discussed. It is anticipated that this review could provide a panoramic sketch and future directions towards the construction of novel artificial ion channels with novel functions and biomedical applications.

Recent Development of Bio-inspired Porous Materials for Catalytic Applications

TANG Yongquan, QI Ganggang, WANG Sai, MENG Xiangju, XIAO Feng-Shou

2023, 39(1): 13-18. doi:10.1007/s40242-022-2164-0

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Nature has served as a source of inspiration for chemists to design the catalysts with superior performance via mimicking their characteristics, such as active sites, reaction microenvironment and electron transfer behaviors. Over a few decades, many different types of materials have been widely used to construct the biomimetic catalysts. Among these materials, the porous materials have been demonstrated to be powerful platforms for constructing the biomimetic catalysts owing to their high surface area, controllable composition and easy functionalization. In this review, we briefly showed recent advances in the construction of various biomimetic porous catalysts using porous materials for the design of excellent catalysts. In addition, we also present the challenge and opportunities in this emerging field.

Recent Progress of Bio-inspired Camouflage Materials: From Visible to Infrared Range

BU Xiaochen, BAI Hao

2023, 39(1): 19-29. doi:10.1007/s40242-022-2170-2

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The adaptability of biological organisms to the environment is reflected in many aspects, especially in their camouflage of appearance. Inspired by biological camouflage strategies, a number of adaptive camouflage materials and devices have been developed to protect soldiers, vehicles, or equipment in the military. Today, the need for adaptive camouflage extends into people’s lives, whose privacy and information security need to be protected in the era of big data. Herein, a review is provided on the recent advancements of adaptive camouflage from the perspective of biological organisms and bio-inspired materials. Firstly, according to different biological mechanisms, we review the typical organisms that use pigmentary color, structural color, and morphological variation for adaptive camouflage, as well as those combine these strategies. Then, we provide an up-to-date review on recent developments in bio-inspired adaptive camouflage materials and devices with an emphasis on visible, infrared, and multispectral camouflage. At last, this review concludes the challenges and prospects for the future development of adaptive camouflage materials. It is noteworthy that there is never the best camouflage. To counter advanced detection techniques, it is necessary to unremittingly develop new materials and technologies to meet the increasing need for adaptive camouflage.

Bioinspired Strategies for Stretchable Conductors

ZHANG Feilong, CHEN Xiaodong

2023, 39(1): 30-41. doi:10.1007/s40242-022-2236-1

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Stretchable conductors are indispensable components of stretchable electronic devices, such as stretchable sensors, transistors, light-emitting diode arrays, solar cells, and so on. However, most of the conductive materials are stiff with very low stretchability. Nature has evolved various strategies to realize stretchability, which give a lot of inspirations to the design and fabrication of stretchable conductors. We herein summarized the nature’s strategies to realize stretchability and revealed the underlying mechanisms. After that, the applications of these strategies in fabricating stretchable conductors are exemplified and the effects of some important parameters on the performances are discussed. Then, possible applications of these stretchable conductors are summarized. Finally, critical issues in the stretchable conductors are discussed and several prospective exploration directions are provided.

Construction and Application of DNAzyme-based Nanodevices

WANG Bo, WANG Menghui, PENG Fangqi, FU Xiaoyi, WEN Mei, SHI Yuyan, CHEN Mei, KE Guoliang, ZHANG Xiao-Bing

2023, 39(1): 42-60. doi:10.1007/s40242-023-2334-8

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The development of stimuli-responsive nanodevices with high efficiency and specificity is very important in biosensing, drug delivery, and so on. DNAzymes are a class of DNA molecules with the specific catalytic activity. Owing to their unique catalytic activity and easy design and synthesis, the construction and application of DNAzymes-based nanodevices have attracted much attention in recent years. In this review, the classification and properties of DNAzyme are first introduced. The construction of several common kinds of DNAzyme-based nanodevices, such as DNA motors, signal amplifiers, and logic gates, is then systematically summarized. We also introduce the application of DNAzyme-based nanodevices in sensing and therapeutic fields. In addition, current limitations and future directions are discussed.

Biomimetic Construction of the Enamel-like Hierarchical Structure

SONG Haoyue, LIU Zhuanfei, ZOU Zhaoyong

2023, 39(1): 61-71. doi:10.1007/s40242-023-2336-6

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Enamel, the hardest mineralized tissue of vertebrates, exhibits simultaneously high stiffness, hardness, and viscoelasticity. The excellent mechanical properties of enamel originate from its high inorganic content and intricate hierarchical structure. Biomimetic construction of the enamel-like hierarchical structure has attracted widespread interest during the past decades. This review summarizes recent advances in this area with a special focus on fabrication techniques across different levels of hierarchy. This includes the synthesis of apatite nanorods or nanowires, the basic building block of enamel, the fabrication of oriented apatite nanorod arrays and the construction of the enamel-like multi-level hierarchical structure. Moreover, possible directions of future research and development in this field are proposed.

Enzymes in Nanomedicine for Anti-tumor Therapy

ZHOU Tong, YUAN Shuaiqi, QIAN Pinrong, WU Yuzhou

2023, 39(1): 72-82. doi:10.1007/s40242-023-2349-1

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Natural enzymes are biological macromolecules catalyzing reactions in living organisms and regulating biological processes. Targeted delivery of enzymes into tumor tissues for anti-tumor therapy through nanotechnology has attracted emerging interest in recent years. In this paper, we systematically summarize the latest research progress on enzymes that used for anti-tumor therapy in nanomedicine with different action mechanisms, including anti-tumor principles, delivery modes, response modes, and synergistic therapeutic design of these enzymes. Finally, we discuss the challenges and future prospects of enzymes for anti-tumor nanomedicine.

Functional Peptides from One-bead One-compound High-throughput Screening Technique

YAN Yaqiong, WANG Lei, WANG Hao

2023, 39(1): 83-91. doi:10.1007/s40242-023-2356-2

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Combinatorial chemistry provides a cost-effective method for the rapid discovery of new functional peptides. One-bead one-compound(OBOC) high-throughput screening technique offers a lot of structurally diverse peptides to be rapidly synthesized and screened for binding to a target of interest. The OBOC peptide library screening involves three main steps: library construction, positive beads separation, and peptide sequencing. This review mainly summarizes some special technique tips during functional peptide screening and potential future directions of the OBOC high-throughput screening technique.

Engineering Mechanical Strong Biomaterials Inspired by Structural Building Blocks in Nature

LI Jiahe, MA Chao, ZHANG Hongjie, LIU Kai

2023, 39(1): 92-106. doi:10.1007/s40242-023-2357-1

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The intricate multiscale architectures in natural structural building blocks provide many sources of inspiration for the designs of artificial biomaterials. In nature, the assembly of highly ordered molecular crystals and amorphous aggregates often derives from inter- and intra-molecular interactions of biomacromolecules, e.g., proteinaceous materials. The structural biomaterials derived from the protein self-assembly behave with remarkable mechanical performance. However, there is still a grand challenge to mimic the mechanical properties of natural protein-based biomaterials in a rational design fashion to yield comparable man-made synthetic ensembles. In this review, a brief perspective on current challenges and advances in terms of bioinspired structural materials is presented. We outline a framework for mimicking protein self-assembly of natural building blocks across multiscale and highlight the critical role of synthetic biology and chemical modifications in material biosynthesis. Particularly, we focus on the design and promising applications of protein-based fibers, adhesives, dynamic hydrogels and engineered living materials, in which natural mechanical functions are effectively reproduced.

Superhydrophobicity-improved Ethanol-Water Separation

XU Lei, CHEN Linfeng, XIA Fan

2023, 39(1): 107-108. doi:10.1007/s40242-023-2320-1

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Efficient separation of biofuels from fermentation broths vis pervaporation plays an important role in addressing the global challenges, such as developing renewable energy. Great efforts have been continuously devoted in the past decades to developing high-performance pervaporation membranes. A recent report published in Science by Zhao et al. showed that a superhydrophobic surface could contribute significantly to improving the pervaporation separation of ethanol-water mixture, which will generate broad interest for the new design of separation membranes.

A Robust Wood-inspired Catalytic System for Highly Efficient Reduction of 4-Nitrophenol

WANG Zeyu, LONG Fei, GAO Huailing, YU Shuhong

2023, 39(1): 109-114. doi:10.1007/s40242-023-2338-4

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Porous solid scaffolds play key roles in preventing nanocatalysts from agglomeration, greatly maintaining the catalytic efficiency and stability of nanocatalysts. However, facile preparation of robust scaffolds with high mass transfer efficiency for loading nanocatalysts remains a major challenge. Here, we fabricate a wood-inspired shape-memory chitosan scaffold for loading Au nanoparticles to reduce 4-nitrophenol via a simple “freeze-casting and dip-adsorption” approach. The obtained catalytic scaffold highly resembles the unidirectional microchannel structure of natural wood, resulting in robust mechanical properties and outstanding water absorption capacity. Additionally, Au nanoparticles can be firmly and uniformly anchored on the inner surface of these microchannels via electrostatic interaction, forming numerous microreactors. This catalytic system exhibits a high 4-nitrophenol conversion rate of 99% in 5 s and impressive catalytic stability even after continuously treating with more than 3 L of highly concentrated 4-nitrophenol solution(1 mmol/L). Therefore, the wood-like catalytic system presented here demonstrates the potential to be applied in the field of water treatment and environmental protection.

Preparation of Photo-responsive DNA Supramolecular Hydrogels and Their Application as UV Radiometers

DING Yuqiao, LI Yujie, YANG Bo, PAN Yufan, CHENG Jiafeng, MENG Siwen, LIU Dongsheng, XU Lijin, DONG Yuanchen

2023, 39(1): 115-120. doi:10.1007/s40242-023-2329-5

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Ultraviolet light(UV) is an essential component of ambient light, but high dose UV would damage genome DNA. While semiconductors and soft materials have been employed to detect the UV, the complex process and the instrumental requirement have limited the application in daily life. In this study, taking advantage of sequence designability, a series of hydrogels with different gel-sol transition rates was constructed under the same UV intensity by introducing competing hybridization to tune the stability of the molecular network. Through estimating the transition time between each system under UV light irradiation, the intensity of UV could be roughly estimated, which provided a convenient method for the visual detection of UV.

Organic Memristor Based on High Planar Cyanostilbene/Polymer Composite Films

ZHAO Jinjin, LI Wei, WANG Xuechen, WEI Xiao, ZHU Huiwen, QU Wenshan, MEN Dandan, GAO Zhixiang, WEI Bin, GAO Hanfei, WU Yuchen

2023, 39(1): 121-126. doi:10.1007/s40242-023-2352-6

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Organic memristors with low power consumption, fast write/erasure speed, and complementary metal-oxide-semiconductor(CMOS) compatibility have attracted tremendous attention to mimic biological synapses to realize neuromorphic computation in recent years. In this paper, organic resistive switching memory(ORSM) based on (Z)-3-(naphthalen-2-yl)-2-(4-nitrophenyl)acrylonitrile(NNA) and polymer poly(N-vinylcarbazole)(PVK) composite film was prepared by spin-coating method. Device performance based on NNA:PVK composite films with different mass fractions of NNA were systematically investigated. The ORSM based on PVK:40%(mass fraction) NNA composite film exhibited non-volatile and bipolar memory properties with a switching ratio(I_on/I_off) of 24.1, endurance of 68 times and retention time of 10⁴ s, a “SET” voltage(V_set) of -0.55 V and a “RESET” voltage(V_reset) of 2.35 V. The resistive switching was ascribed to the filling and vacant process of the charge traps induced by NNA and the inherent traps in PVK bulk. The holes trapping and de-trapping process occurred when the device was applied with a negative or positive bias, which caused the transforming of the conductive way of charges, that is the resistive behaviors in the macroscopic. This study provides a promising platform for the fabrication of ORSM with high performance.

Scalable and Robust Bio-inspired Organogel Coating by Spraying Method Towards Dynamic Anti-scaling

ZANG Ruhua, CHEN Zijia, YANG Hui, WANG Yixuan, WANG Shutao, MENG Jingxin

2023, 39(1): 127-132. doi:10.1007/s40242-022-2094-x

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Scaling usually causes serious problems in daily life and industrial production. Currently, developing passive anti-scaling coatings has shown promises to overcome this problem. In this work, we fabricated a scalable and robust bio-inspired organogel(BIO) coating, showing dynamic scale resistance in the oil/brine mixture. The oil layer of the BIO coating was utilized as a barrier to inhibit scale nucleation and reduce scale adhesion. The mechanical strength of the coating was optimized by regulating nanoparticle contents. Moreover, the universality of scale resistance was demonstrated by varying the types of nanoparticles, oils and scales. Compared with commercial pipeline materials, such as copper, this BIO coating significantly reduces scale deposition after 240-h scaling test(ca. 93% reduction). Therefore, this study designs scalable and robust organogel coatings for sustainable scale resistance, which may be used for practical application in oil production.

Transpiration-inspired Capillary for Synchronous Synthesis and Patterning of Silver Nanoparticles

CHEN Bingda, ZHANG Zelong, SU Meng, QIN Feifei, PAN Qi, XIE Daixi, YANG Xu, ZHANG Kun, ZHANG Zeying, XIE Hongfei, CARMELIET Jan, SONG Yanlin

2023, 39(1): 133-138. doi:10.1007/s40242-023-2325-9

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Traditional synthesis strategy of nanomaterials with complicated process and high cost limits their applications. Here, we propose a facile process for the synchronous synthesis and patterning of silver nanoparticles(Ag NPs) through the self-driven microchannel reactor with the capillary effect inspired by transpiration. The evaporation contributes to capillary and accumulation effects in the microchannels. The silver reactant-containing droplets can be spontaneously divided and distributed in multiple microchannels during the whole fabrication process by the capillary effect. The newly formed Ag NPs at the gas-liquid interface can be assembled on both sides of the microchannels by the accumulation effect. The capillary effect decreases the disturbances, which ensures the uniformity of the patterning. By the combination of microchannels with different widths, various Ag NPs-assembled patterns with stable electrical properties are achieved. This efficient strategy with a simple fabrication procedure is towards the technological engineering of nanoscale architected materials.

Chemically Amplified Resist Based on Dendritic Molecular Glass for Electron Beam Lithography

HU Shengwen, CHEN Jinping, YU Tianjun, ZENG Yi, YANG Guoqiang, LI Yi

2023, 39(1): 139-143. doi:10.1007/s40242-022-2163-1

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A novel dendritic molecular glass(MG) containing adamantane core(AD-15) was synthesized and characterized. It exhibits good solubility in common organic solvents and a stable amorphous state at room temperature, which contributes to forming films with different thicknesses by spin-coating. The thermal analysis of AD-15 indicates that no apparent glass transition temperature(T_g) is observed before the thermal decomposition temperature(T_d=160 ℃). The good thermal resistance suggests that it can satisfy the lithographic process and is a candidate for photoresist materials. The patterning properties of AD-15 resist were evaluated by electron beam lithography(EBL). By optimizing the lithographic process parameters, AD-15 resist can achieve 40 nm half-pitch patterns with a line-edge roughness of 4.0 nm. The contrast and sensitivity of AD-15 resist were 1.9 and 67 μC/cm², respectively. Compared with the commercial PMMA(950k) electron beam resist, the sensitivity of AD-15 resist increases by 6 times. This study provides a new example of molecular glass resist with high resolution and sensitivity for EBL.

Nucleotide Recognition by a Guanidinocalixarene Receptor in Aqueous Solution

GENG Wenchao, ZHENG Zhe, JIANG Huifeng, GUO Dongsheng

2023, 39(1): 144-150. doi:10.1007/s40242-022-2204-9

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Nucleotides participate in various physiological processes through their supramolecular interactions with biomolecules. Therefore, the molecular recognition of nucleotides became an important topic in supramolecular chemistry and exhibited many biomedical applications. Guanidinocalixarenes showed very strong binding affinities towards nucleotides, even reaching the nanomolar level. In this work, we systematically determined the binding constants between a typical guanidinocalixarene(guanidinium-modified calix[5]arene, GC5A) and various nucleotides and revealed the driving forces behind the molecular recognition using theoretical calculations. The electrostatic interactions and hydrogen bonding provided by the phosphate groups of the nucleotides dominated the binding between the nucleotides and GC5A. The lower rim alkyl chains and the skeleton of GC5A provide preorganized cavity and upper guanidinium groups. The difference in the type of nucleobase is also attributed to the different binding affinities. This work provides insight into the molecular recognition of nucleotides and facilitates the development of new supramolecular hosts for nucleotides and related biological applications.

Smart Multiple Wetting Control on ZnO Coated Shape Memory Polymer Arrays

WANG Xiaonan, WANG Bohan, LAI Hua, CHENG Zhongjun

2023, 39(1): 151-158. doi:10.1007/s40242-022-2265-9

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Recently, surfaces with intelligent wetting controllability have aroused increased attention. Endowing the surface with stimuli-responsive surface chemistry and tunable surface microstructure can achieve a surface with smart wetting performances. However, almost all existing surfaces only focused on single surface chemistry or micromorphology, thus to achieve smart multiple wetting regulation is still difficult. Herein, we report a ZnO coated shape memory polymer(SMP) surface, and the surface chemistry and micromorphology can be synergistically regulated. ZnO can provide adjustable surface chemistry under UV irradiation, and SMP can offer tunable micromorphology due to its shape memory effect(SME). Based on the combined effect between the above two features, surface wetting performance can be smartly regulated among multiple states. Moreover, due to the excellent controllability of the surface, the application in directional droplet transportation was also demonstrated. This paper offers a new surface with tunability in both surface chemistry and micromorphology, and given the excellent wetting controllability, the surface is believed to be applied in a lot of fields, such as droplet manipulation, fluidic devices and selective catalysis.

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