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Photo-Driven Ammonia Synthesis via a Proton-Mediated Photoelectrochemical Device

Angewandte Chemie 2025年第8期137卷

作者： Wan Lin Jiajie Chen Xiang Zhang Jing Lin Fuwen Lin ShenXia Huang Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Fujian College University of Chinese Academy of Sciences Fuzhou 350002 P. R. China College of Chemistry Fuzhou University Fuzhou 350116 Fujian P. R. China. Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China College of Chemistry and Materials Science Fujian Normal University Fuzhou 350007 China

N 2 reduction reaction (NRR) by light is an energy-saving and sustainable ammonia (NH 3 ) synthesis technology. However, it faces significant challenges, including high energy barriers of N 2 activation and unclear catalytic active sites. Herein, we propose a strategy of photo-driven ammonia synthesis via a proton-mediated photoelectrochemical device. We used redox-catalysis covalent organic framework (COF), with a redox site (−C=O) for H + reversible storage and a catalytic site (porphyrin Au) for NRR. In the proton-mediated photoelectrochemical device, the COF can successfully store e − and H + generated by hydrogen oxidation reaction, forming COF−H. Then, these stored e − and H + can be used for photo-driven NRR (108.97 umol g −1 ) under low proton concentration promoted by the H-bond network formed between −OH in COF−H and N 2 on Au, which enabled N 2 hydrogenation and NH 3 production, establishing basis for advancing artificial photosynthesis and enhancing ammonia synthesis technology.

关键词： Photo-driven ammonia synthesis Proton-mediated N2 reduction reaction Covalent organic framework Photoelectrochemical device

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A Photoresponsive Battery Based on a Redox-Coupled Covalent-Organic-Framework Hybrid Photoelectrochemical Cathode

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Angewandte Chemie 2022年第50期134卷

作者： Wei Wang Dr. Xiang Zhang Dr. Jing Lin Dr. Lei Zhu Enbo Zhou Dr. Yangyang Feng Prof. Daqiang Yuan Prof. Yaobing Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 Fujian P. R. China

Photoresponsive batteries promise flexible and low-cost solar-to-electrochemical energy storage (SES), but suffer from a limited SES efficiency due to rapid charge recombination and sluggish redox. Here, we present a porous-shell/core hybrid of covalent organic framework@carbon nanotube. This hybrid ensures long-lived separated charges (τ ave =3.0 ns) by an electron transfer relay starting from the donor-acceptor molecules to the nanoscale heterojunction. These charges are further allowed to drive high-rate redox of −C=O/−C−O − and −C−N/−C=N + with facile kinetics. Equipped with this photoelectrochemical cathode, a photoresponsive aqueous battery shows a 5-fold enhancement in SES efficiency (1.1 % at 1 sun) over their counterparts. It is unveiled that the electron relay favors the formation of electron-enriching −C−O− and hole-enriching −C=N + groups responsible for photoelectrochemical Zn 2+ and OTf − storage cascade; and further, the general photo coupled ions transfer (PCIT) process is proposed. This work presents an inspiring photoelectrochemical cathode design and theoretical insight for photoresponsive batteries.

关键词： Core–Shell Hybrid Materials Covalent Organic Frameworks Photo Coupled Ions Transfer (PCIT) Photoelectrochemistry Photoresponsive Batteries

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Boosting Near-Infrared Luminescence of Lanthanide in Cs2AgBiCl6Double Perovskites via Breakdown of the Local Site Symmetry

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Angewandte Chemie 2022年第30期134卷

作者： Yifan Pei Prof. Datao Tu Chenliang Li Siyuan Han Dr. Zhi Xie Fei Wen Luping Wang Prof. Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China College of Chemistry and Materials Science Fujian Normal University Fuzhou Fujian 350117 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China College of Mechanical and Electronic Engineering Fujian Agriculture and Forestry University Fuzhou Fujian 350002 China

Currently, lanthanide (Ln 3+ )-doped near-infrared (NIR)-emitting double perovskites (DPs) suffer from low photoluminescence quantum yield (PLQY). Herein, we develop a new class of NIR-emitting DPs based on Ln 3+ -doped Cs 2 (Na/Ag)BiCl 6 . Benefiting from the Na + -induced breakdown of local site symmetry in the Cs 2 AgBiCl 6 DPs, effective NIR emissions of Ln 3+ are realized through Bi 3+ sensitization. Specifically, 7.3-fold and 362.9-fold enhanced NIR emissions of Yb 3+ and Er 3+ are achieved in Cs 2 Ag 0.2 Na 0.8 BiCl 6 DPs relative to those in Na-free Cs 2 AgBiCl 6 counterparts, respectively. The optimal absolute NIR PLQYs for Yb 3+ and Er 3+ in Cs 2 Ag 0.2 Na 0.8 BiCl 6 DPs are determined to be 19.0 % and 4.3 %, respectively. Raman spectroscopy and first-principles density functional theory calculations verify the sublattice distortion in Cs 2 (Na/Ag)BiCl 6 DPs via Na + doping. These findings provide fundamental insights into the design of efficient NIR-emitting Ln 3+ -doped DPs for versatile optoelectronic applications.

关键词： Cs2AgBiCl6 Double Perovskites Lanthanide Ions Local Site Symmetry Near-Infrared Luminescence

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From a Metal–Organic Square to a Robust and Regenerable Supramolecular Self-assembly for Methane Purification

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Angewandte Chemie 2022年第48期134卷

作者： Zhong-Min Cao Dr. Guo-Ling Li Dr. Zheng-Yi Di Dr. Cheng Chen Prof. Dr. Ling-Yi Meng Prof. Dr. Mingyan Wu Prof. Dr. Wei Wang Dr. Zhu Zhuo Prof. Dr. Xiang-Jian Kong Prof. Dr. Maochun Hong Prof. Dr. You-Gui Huang CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institutes Chinese Academy of Sciences Xiamen Fujian 361021 China State Key Laboratory of Structure Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China State Key Laboratory of Physical Chemistry of Solid Surfaces Xiamen University Xiamen Fujian 361005 China

Porous supramolecular assemblies constructed by noncovalent interactions are promising for adsorptive purification of methane because of their easy regeneration. However, the poor stability arising from the weak noncovalent interactions has obstructed their practical applications. Here, we report a robust and easily regenerated polyhedron-based cationic framework assembled from a metal–organic square. This material exhibits a very low affinity for CH 4 and N 2 , but captures other competing gases (e.g. C 2 H 6 , C 3 H 8 , and CO 2 ) with a moderate affinity. These results underpin highly selective separation of a range of gas mixtures that are relevant to natural gas and industrial off-gas. Dynamic breakthrough studies demonstrate its practical separation for C 2 H 6 /CH 4 , C 3 H 8 /CH 4 , CO 2 /N 2 , and CO 2 /CH 4 . Particularly, the separation time is ≈11 min g −1 for the C 2 H 6 /CH 4 (15/85 v/v) mixture and ≈49 min g −1 for the C 3 H 8 /CH 4 (15/85 v/v) mixture (under a flow of 2.0 mL min −1 ), respectively, enabling its capability for CH 4 purification from light alkanes.

关键词： Alkanes Separation CO2 Capture Metal–Organic Square Polyhedral Cavity Supramolecular assembly

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High‐Voltage Rechargeable Alkali–Acid Zn–PbO2 Hybrid Battery

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Angewandte Chemie 2020年第52期132卷 23799-23803页

作者： Yunpeng Xu Pingwei Cai Kai Chen Yichun Ding Prof. Long Chen Weifan Chen Prof. Dr. Zhenhai Wen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 P. R. China Department of Chemistry Institute of Molecular Plus Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin University Tianjin 300072 P. R. China University of Chinese Academy of Science Beijing 100049 P. R. China School of Materials Science & Engineering Nanchang University Nanchang 330031 P. R. China

An alkaline–acid Zn‐PbO2 hybrid battery is developed by coupling a zinc alkaline anode with an acidic PbO2 cathode. The system gives a high desirable electrochemical performance with high working voltage, high area capacity, and long cyclic stability. The present system addresses some of the critical problems of traditional aqueous batteries (e.g., lead acid batteries).Aqueous rechargeable batteries have attracted attention owning to their advantages of safety, low cost, and sustainability, while the limited electrochemical stability window (1.23 V) of water leads to their failure in competition with organic‐based lithium‐ion batteries. Herein, we report an alkali–acid Zn–PbO2 hybrid aqueous battery obtained by coupling an alkaline Zn anode with an acidic PbO2 cathode. It shows the capability to deliver an impressively high open‐circuit voltage (Voc) of 3.09 V and an operate voltage of 2.95 V at 5 mA cm−2, thanks to the contribution of expanding the voltage window and the electrochemical neutralization energy from the alkali–acid asymmetric‐electrolyte hybrid cell. The hybrid battery can potentially deliver a large area capacity over 2 mAh cm−2 or a high energy density of 252.39 Wh kg−1 and shows almost no fading in area capacity over 250 charge–discharge *** a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re‐organized for online delivery, but are not copy‐edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the *** note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

关键词： alkali-acid electrolytes aqueous batteries high voltage rechargeable Zn-PbO2 battery

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Nanoporous Single-Crystalline Oxide Catalysts for Preferential Oxidation of CO in H2with an Ultra-wide Temperature Window

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Angewandte Chemie 2022年第50期134卷

作者： Wenting Li Prof. Kui Xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China Key Laboratory of Design & Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China

Preferential oxidation of CO in H 2 (PROX) reaction is a promising solution to the on-board purification of CO-contaminated H 2 fuel for use in next-generation proton-exchange membrane fuel cells (PEMFC). However, achieving high CO selectivity, activity and structural stability across the wide temperature window remains a great challenge. Herein, we fabricate centimeter scale interfacial PROX catalysts grown from nanoporous single-crystalline Pr 2 O 3 and Nd 2 O 3 monoliths with lattice surface-deposited Pt clusters at nanoscale. We demonstrate complete and selective removal of CO in H 2 over an unprecedented wide temperature window (253–403 K). The monoliths are integrated with an operational PEMFC to purify the H 2 fuel contaminated with CO (30 ppm) and enable stable power output for >400 h; over two thousand times longer than without. This work demonstrates that the nanoporous single-crystalline oxide monoliths can simultaneously achieve the stability and overall performance required to realize practically useful PEMFCs.

关键词： Porosity Preferential Oxidation Pt Cluster Single Crystal

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Multifunctional ternary entropy-regulatory RE 2 W 2 O 9 (RE = Ce, Gd, Ho) yellow pigments: high near-infrared reflectance, anti-ultraviolet aging, and antimycotic performance

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Journal of Rare Earths 2025年

作者： Haiying Xin Liyan Xue Mengtong Ma Ke Song Qiyong Deng Zhiyi Wang Minzhong Huang Fan Yang College of Chemistry Fuzhou University Fuzhou 350108 China Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 China Fujian College University of Chinese Academy of Sciences Fuzhou 350002 China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 China Fujian Province Joint Innovation Key Laboratory of Fuel and Materials in Clean Nuclear Energy System Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China China Rare Earth Group Research Institute Shenzhen 518000 China Key Laboratory of Rare Earths Ganjiang Innovation Academy Chinese Academy of Sciences Ganzhou 341000 China

To mitigate the urban heat island effect, align with the “double carbon strategy”, and address the issues of coating aging and mildew on building facades, multifunctional ternary entropy-regulatory tungstate ceramic cool pigments (Ce x Ho 0.1 Gd 1.9– x W 2 O 9+ δ ) were prepared by high-temperature solid-phase method in this study. While ensuring the high near-infrared (NIR) solar reflectance, the anti-ultraviolet (UV) aging and antimycotic performance of rare earth given to pigment were evaluated, and its optical properties, microstructure and practical application effects were deeply explored. The results indicate that ternary entropy regulation changes the color of the pigment from white to yellow, significantly reducing the band gap from 3.28 to 1.90–1.87 eV. Specifically, the Ce 0.2 Ho 0.1 Gd 1.7 W 2 O 9+ δ pigment exhibits excellent chromatic properties ( L * = 73.79, a * = 20.21 and C * = 50.51) and a high NIR solar reflectance (96.23%). Infrared thermography confirms that it has a good cooling effect, with temperatures of 3.5 °C lower than the commercially available coating of similar color. Furthermore, the performance of multifunctional integration is that the pigments show enhanced absorption in the UVA (long-wave ultraviolet 320–400 nm) range, with an increase in average light absorption from 0.19 to 0.91 and a substantial increase in antimycotic rate from 42.86% to 97.46%. At the same time, this material has good acid and alkali resistance (Δ E * ≤ 2.41). The successful development of the multifunctional cool pigment materials opens a new way to energy-saving architectural wall coating materials.

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In situ Observation of Porosity Formation in Porous Single-crystalline TiO2Monolith for Enhanced and Stable Catalytic CO Oxidation

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Angewandte Chemie 2023年第12期135卷

作者： Fangyuan Cheng Jie Zhang Prof. Kui Xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou Guangdong 116023 China University of Chinese Academy of Sciences Beijing 100049 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China Key Laboratory of Design & Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China

Introducing pores in single crystals creates a new type of porous materials that incorporate porosity and structural coherence. Herein, we use in situ transmission electron microscopy to disclose the porosity formation by converting KTiOPO 4 (KTP) single crystals into porous single-crystalline (PSC) TiO 2 monoliths in a solid-solid transformation. The isolated crystalline nuclei of TiO 2 clusters with identical lattice orientation on KTP surface moves TiO 2 /KTP interface toward mother phase for growing PSC TiO 2 monoliths. The relative density in PSC TiO 2 monoliths dominates porosity while the macroscopic dimensions remain unchanged in the transformation. The single-crystalline nature of porous architecture stabilizes oxygen vacancy to activate lattice oxygen while the three-dimensional percolation enhances species diffusion. PSC TiO 2 monoliths with deposited Pt clusters show enhanced and stable catalytic CO oxidation in air at ∼75 °C for 200 hours of operation.

关键词： Porous single crystal TiO2 In situ TEM Solid-solid transformation CO oxidation

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Single-atom Iron Catalyst with Biomimetic Active Center to Accelerate Proton Spillover for Medical-level Electrosynthesis of H2O2Disinfectant

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Angewandte Chemie 2023年第34期135卷

作者： Dr. Yan Li Dr. Junxiang Chen Yaxin Ji Zilin Zhao Wenjun Cui Dr. Xiahan Sang Dr. Yi Cheng Dr. Bin Yang Dr. Zhongjian Li Dr. Qinghua Zhang Prof. Dr. Lecheng Lei Prof. Dr. Zhenhai Wen Prof. Dr. Liming Dai Prof. Dr. Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University 310027 Hangzhou China Center of Advanced Carbon Materials School of Chemical Engineering University of New South Wales 2052 Sydney NSW Australia CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences 350002 Fuzhou Fujian China Research and Testing Centre of Material School of Materials Science and Engineering Wuhan University of Technology 430070 Wuhan China Zhejiang Hengyi Petrochemical Research Institute Co. Ltd. 311200 Hangzhou China Institute of Zhejiang University—Quzhou 324000 Quzhou China Donghai Laboratory 316021 Zhoushan China

Electrosynthesis of H 2 O 2 has great potential for directly converting O 2 into disinfectant, yet it is still a big challenge to develop effective electrocatalysts for medical-level H 2 O 2 production. Herein, we report the design and fabrication of electrocatalysts with biomimetic active centers, consisting of single atomic iron asymmetrically coordinated with both nitrogen and sulfur, dispersed on hierarchically porous carbon (Fe SA -NS/C). The newly-developed Fe SA -NS/C catalyst exhibited a high catalytic activity and selectivity for oxygen reduction to produce H 2 O 2 at a high current of 100 mA cm −2 with a record high H 2 O 2 selectivity of 90 %. An accumulated H 2 O 2 concentration of 5.8 wt.% is obtained for the electrocatalysis process, which is sufficient for medical disinfection. Combined theoretical calculations and experimental characterizations verified the rationally-designed catalytic active center with the atomic Fe site stabilized by three-coordinated nitrogen atoms and one-sulfur atom (Fe-N 3 S-C). It was further found that the replacement of one N atom with S atom in the classical Fe-N 4 -C active center could induce an asymmetric charge distribution over N atoms surrounding the Fe reactive center to accelerate proton spillover for a rapid formation of the OOH* intermediate, thus speeding up the whole reaction kinetics of oxygen reduction for H 2 O 2 electrosynthesis.

关键词： H2O2 Production Medical-Level Disinfectant Fe Single Atom Proton Spillover Promoted Reaction Kinetics

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Engineering the Bandgap and Surface Structure of CsPbCl3Nanocrystals to Achieve Efficient Ultraviolet Luminescence

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Angewandte Chemie 2021年第17期133卷

作者： Yunqin Zhang Dr. Xiyue Cheng Dr. Datao Tu Dr. Zhongliang Gong Renfu Li Yingjie Yang Prof. Wei Zheng Dr. Jin Xu Prof. Dr. Shuiquan Deng Prof. Dr. Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China University of Chinese Academy of Sciences Beijing 100049 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China

Herein, we report the design of novel ultraviolet luminescent CsPbCl 3 nanocrystals (NCs) with the emission peak at 381 nm through doping of cadmium ions. Subsequently, a surface passivation strategy with CdCl 2 is adopted to improve their photoluminescence quantum yield (PLQY) with the maximum value of 60.5 %, which is 67 times higher than that of the pristine counterparts. The PLQY of the surface passivated NCs remains over 50 % after one week while the pristine NCs show negligible emission. By virtue of density functional theory calculations, we reveal that the higher PLQY and better stability after surface passivation may result from the significant elimination of surface chloride vacancy (V Cl ) defects. These findings provide fundamental insights into the optical manipulation of metal ion-doped CsPbCl 3 NCs.

关键词： band gap CsPbCl3 lead halide perovskite nanocrystals surface passivation ultraviolet luminescence

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