【最新中稿作品】寡聚吡咯笼类功能分子系统、光电/铁电晶体管、钙钛矿太阳能电池等

中稿作品 · 解读

题目：Oligopyrrolic Cages: From Classic Molecular Constructs to Chemically Responsive Polytopic Receptors

作者：Fei Wang, Christophe Bucher, Qing He*, Atanu Jana*, and Jonathan L. Sessler*

引用：Acc. Chem. Res. 2022, 12, 1646–1658.

DOI: 10.1021/acs.accounts.2c00120

“功能分子系统”是一种离散的且可组装的结构，能够实现对分子识别、结构、成键、转运、释放、催化活性等过程的控制，是当前科学研究的热门话题之一。在这一广泛的研究领域中，寡聚吡咯笼类化合物由于其响应性识别特征而备受关注。

近日，湖南大学化学化工学院王飞博士后、何清教授以及德克萨斯大学奥斯汀分校 Jonathan L. Sessler教授等人报道了有关低聚吡咯类笼状结构的最新研究进展评述。该评述总结了团队近年来有关（1）共价低吡咯类分子笼、（2）低聚吡咯金属笼以及（3）低聚吡咯非共价笼的合成、结构、性质及其选择性客体识别和封装、阴离子结合和离子通道、气体吸收等应用的最新研究进展。本报告重点介绍了我们团队对离散的低聚吡咯类大环化学的贡献，以及它们在超分子主客体化学和传感中的应用。希望该报告能够为了解低聚吡咯笼化学提供基础，对基于吡咯基元的功能分子系统设计研究提供指导，从而推动该领域的进一步发展。期刊Accounts of Chemical Research（IF: 22.384）在线发表该评述文章——Oligopyrrolic Cages: From Classic Molecular Constructs to Chemically Responsive Polytopic Receptors（Acc. Chem. Res. 2022, 12, 1646–1658. DOI: 10.1021/acs.accounts.2c00120），并被选为期刊封面文章。

中稿封面 · 一周精选

1

丨Vol.34 No.23 June 9,2022

标题Title

Negative Phototransistors with Ultrahigh Sensitivity and Weak-Light Detection Based on 1D/2D Molecular Crystal p–n Heterojunctions and their Application in Light Encoders (Adv. Mater. 23/2022)

摘要Abstract（滑动查看）

Anomalous negative phototransistors in which the channel current decreases under light illumination hold potential to generate novel and multifunctional optoelectronic applications. Although a variety of design strategies have been developed to construct such devices, NPTs still suffer from far lower device performance compared to well-developed positive phototransistors (PPTs). In this work, a novel 1D/2D molecular crystal p–n heterojunction, in which p-type 1D molecular crystal (1DMC) arrays are embedded into n-type 2D molecular crystals (2DMCs), is developed to produce ultrasensitive NPTs. The p-type 1DMC arrays act as light-absorbing layers to induce p-doping of n-type 2DMCs through charge transfer under illumination, resulting in ineffective gate control and significant negative photoresponses. As a result, the NPTs show remarkable performances in photoresponsivity (P) (1.9 × 108) and detectivity (D*) (1.7 × 1017 Jones), greatly outperforming previously reported NPTs, which are one of the highest values among all organic phototransistors. Moreover, the device exhibits intriguing characteristics undiscovered in PPTs, including precise control of the threshold voltage by controlling light signals and ultrasensitive detection of weak light. As a proof-of-concept, the NTPs are demonstrated as light encoders that can encrypt electrical signals by light. These findings represent a milestone for negative phototransistors, and pave the way for the development of future novel optoelectronic applications.

封面论文链接：

https://doi.org/10.1002/adma.202270174

2

丨Vol.32 No.25 June 17,2022

标题Title

Enhanced Piezoelectric Properties and Improved Property Uniformity in Nd-Doped PMN-PT Relaxor Ferroelectric Single Crystals (Adv. Funct. Mater. 25/2022)

摘要Abstract（滑动查看）

Relaxor-PbTiO3 crystals exhibit excellent piezoelectric properties (d33 > 2000 pC N−1 and k33 > 90%) and thus attractes widespread attention in the past two decades. However, the inevitable segregation of components during the crystal growth results in relatively low-performance consistency of Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) crystals, which seriously affects their practical applications. In this work, Nd3+ as A-site substitution is introduced to improve the uniformity of electromechanical performance of PMN-PT crystal. The results show that the crystal exhibits a high piezoelectric coefficient of 3000 pC N−1 in rhombohedral phase with a variation of 36%. The electron probe X-ray microanalyzer indicates that the opposite separation characteristics of Nd3+ and Ti4+ lead to improved uniformity of piezoelectric performance along the crystal boule. The giant piezoelectricity in Nd-doped PMN-PT is attributed to the enhanced local structural heterogeneity introduced by doping Nd. Furthermore, the Nd-doped PMN-PT crystal shows the rhombohedral-tetragonal phase transition temperature in the range of 74–87 °C, which indicates that Nd-doped PMN-PT crystal can be a promising candidate for the design of advanced piezoelectric transducers.

封面论文链接：

https://doi.org/10.1002/adfm.202270145

3

丨Vol.12 No.26 July 14, 2022

标题Title

Synergistic Structural Engineering of Tunnel-Type Polyantimonic Acid Enables Dual-Boosted Volumetric and Areal Lithium Energy Storage (Adv. Energy Mater. 26/2022)

摘要Abstract（滑动查看）

Tunnel-structured polyantimonic acid (PAA) is an intriguing high-capacity anode candidate for alkali-metal-ion storage; however, the awful electroconductivity of PAA (≈10–10 S cm–1) normally requires coupling with large-surface-area conductive substrate (e.g., graphene), conversely leading to poor scalability, ultralow density, and execrable volumetric energy. Synergistic structural engineering of PAA via bulk-phase ion substitution and incorporation with low-cost flake graphite (FG) is presented here to construct composite electrodes for lithium-storage. The full-occupation of Mn2+ into the tunnel-centers of PAA synchronously improves its bulk conductivity (≈10–5 S cm–1) and true density (4.58 g cm–3), whilst less than 20% volume expansion of PAA is consequently achieved by FG confinement with enhanced multielectron-reaction kinetics, unveiled by ex/in situ techniques. Besides delivering considerable volumetric capacity (>1200 mAh cm–3 at 0.1 A g–1), thus-fabricated high-tap-density composite favors the construction of conducting additive-free, high-loading thick electrodes (>6.0 mg cm–2), exhibiting dual-boosted areal/volumetric capacities (4.2 mAh cm–2/743 mAh cm–3), and fast-charging capability (75% capacity charged within ≈13 min). Moreover, 3D-printed composite electrodes with tunable shape and mass-loading are also implemented to showcase impressive areal/volumetric Li+-storage performance. Paring with high-loading and high-compact-density LiCoO2 cathodes (e.g., 18.0 mg cm–2/3.53 g cc–1), full-cells achieve remarkable electrode-level areal-/volumetric-energy-densities beyond 7.0 mWh cm–2/850 Wh L–1cathode+anode.

封面论文链接：

https://doi.org/10.1002/aenm.202200653

4

丨Vol.4 No.7 July, 2022

标题Title

Strategies for high-performance perovskite solar cells from materials, film engineering to carrier dynamics and photon management

摘要Abstract（滑动查看）

In recent years, halide perovskite solar cells (HPSCs) have attracted a great attention due to their superior photoelectric performance and the low-cost of processing their quality films. In order to commercialize HPSCs, the researchers are focusing on developing high-performance HPSCs. Many strategies have been reported to increase the power conversion efficiency and the long-term stability of HPSCs over the past decade. Herein, we review the latest efforts and the chemical-physical principles for preparing high-efficiency and long-term stability HPSCs in particular, concentrating on the perovskite materials, technologies for perovskite films, charge transport materials and ferroelectric effect to reduce the carrier loss, and photon management via plasmonic and upconversion effects. Finally, the key issues for future researches of HPSCs are also discussed with regard to the requirements in practical application.

封面论文链接：

https://doi.org/10.1002/inf2.12322

5

丨Vol.43 No.6 June, 2022

标题Title

Direct writing-in and visualizing reading-out data storage with high capacity in low-cost plastics

摘要Abstract（滑动查看）

The explosive growth of the global data volume demands new and advanced data storage methods. Here, we report that data storage with ultrahigh capacity (~1 TB per disc) can be realized in low-cost plastics, including polycarbonate (PC), precipitated calcium carbonate (PCC), polystyrene (PS), and polymethyl methacrylate (PMMA), via direct fs laser writing. The focused fs laser can modify the fluorescence of written regions on the surface and in the interior of PMMA, enabling three-dimensional (3D) information storage. Through the 3D laser processing platform, a 50-layer data record with low bit error (0.96%) is archived. Visual reading of data is empowered by the fluorescence contrast. The broad variation of fluorescence intensity assigns 8 gray levels, corresponding to 3 bits on each spot. The gray levels of each layer present high stability after long-term aging cycles, confirming the robustness of data storage. Upon single pulse control via a high-frequency electro-optic modulator (EOM), a fast writing speed (~1 kB/s) is achieved, which is limited by the repetition frequency of the fs laser.

封面论文链接：

https://doi.org/10.1088/1674-4926/43/6/062301

6

丨Vol.13 No.25 June 30, 2022

标题Title

Orbital Dependence in Single-Atom Electrocatalytic Reactions

摘要Abstract（滑动查看）

Transition metal single-atom catalysts supported on N-doped graphene (TM–N–C) could serve as an ideal model for studying orbital dependence in electrocatalytic reactions because the atom on the catalytic active site has discrete single-atom-like orbitals. In this work, the catalytic efficiency of Fe–N–C for the oxygen evolution reaction (OER) under a small structural perturbation has been comprehensively investigated with density functional theory calculations. The results suggest that the subtle local environment of a single atom can significantly modulate the catalytic reactivity. Further analysis demonstrates that the energy level of the TM dz2 orbital center, rather than the d-band center, is responsible for the OER catalytic efficiency as the dz2 orbital participates mainly in the reactions. Essentially, the d-band theory can be extended to the sub-d orbital level, and a small perturbation of the crystal field, induced by lattice strain or z-direction displacement of the TM atom, can prominently change the sub-d orbital associated with the reaction and in turn affect the catalytic activity.

封面论文链接：

https://doi.org/10.1021/acs.jpclett.2c01381

7

丨Vol.8 No.7 July, 2022

标题Title

Transition State Theory-Inspired Neural Network for Estimating the Viscosity of Deep Eutectic Solvents

摘要Abstract（滑动查看）

The lack of accurate methods for predicting the viscosity of solvent materials, especially those with complex interactions, remains unresolved. Deep eutectic solvents (DESs), an emerging class of green solvents, have a severe lack of viscosity data, resulting in their application still staying at the stage of random trial and error, and it is difficult for them to be implemented on an industrial scale. In this work, we demonstrate the successful prediction of the viscosity of DESs based on the transition state theory-inspired neural network (TSTiNet). The TSTiNet adopts multilayer perceptron (MLP) for the transition state theory-inspired equation (TSTiEq) parameters calculation and verification using the most comprehensive DESs viscosity data set to date. For the energy parameters of the TSTiEq, the constant assumption and the fast iteration with the help of MLP can allow TSTiNet to achieve the best performance (the average absolute relative deviation on the test set of 6.84% and R2 of 0.9805). Compared with the traditional machine learning methods, the TSTiNet has better generalization ability and dramatically reduces the maximum relative deviation of prediction under the constraints of the thermodynamic formulation. It requires only the structural information on DESs and is the most accurate and reliable model available for DESs viscosity prediction.

封面论文链接：

https://doi.org/10.1021/acscentsci.2c00157

1

丨Vol.14 No.27 July 21, 2022

标题Title

A pixelated frequency-agile metasurface for broadband terahertz molecular fingerprint sensing

摘要Abstract（滑动查看）

Terahertz (THz) plasmonic resonance based on an arbitrarily designed resonance metasurface is the key technique of choice for enhancing fingerprint absorption spectroscopy identification of biomolecules. Here, we report a broadband THz micro-photonics sensor based on a pixelated frequency-agile metasurface and illustrate its application ability to enhance and differentiate the detection of broadband absorption fingerprint spectra. The design uses symmetrical metal C-shape resonators with the functional graphene micro-ribbons selectively patterned into the gaps. A strong electric resonance with a high quality factor was formed, consisting of an electric dipole mode associated with the excitation of a dark toroidal dipole (TD) mode through the coupling from the electric dipole moment of the individual frequency-agile meta-unit. The resonance positions are nearly linearly modulated with the varying Fermi level of graphene. The configuration arranges a certain metapixel of the metasurface to multiple response spectra assembling a one-to-many mapping between spatial and spectral information which is instrumental in greatly shrinking the actual size of the sensor. By the synchronous regulation of graphene and C-shape rings, we have obtained highly surface-sensitive resonances over a wide spectral range (∼1.5 THz) with a spectral resolution less than 20 GHz. The target multiple enhanced absorption spectrum of glucose molecules is read out in a broadband region with high sensitivity. More importantly, the design can be extended to cover a larger spectral region by altering the range of geometrical parameters. Our microphotonic technique can resolve absorption fingerprints without the need for spectrometry and frequency scanning, thereby providing an approach for highly sensitive and versatile miniaturized THz spectroscopy devices.

封面论文链接：

https://doi.org/10.1039/D2NR01561G

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