Review
Polymer Science
Lei Wang, Hangxun Xu
Summary: This article comprehensively summarizes the recent progress in the development of two-dimensional conjugated polymer frameworks (2D CPFs) for solar fuel generation from water, including the basic principles and structure-property relationships. The article also highlights the applications of 2D CPFs in photoelectrochemical energy conversion and discusses the remaining challenges and research opportunities for the future development.
PROGRESS IN POLYMER SCIENCE
(2023)
Article
Multidisciplinary Sciences
Kai-Kai Chen, Chao-Chao Qin, Meng-Jie Ding, Song Guo, Tong-Bu Lu, Zhi-Ming Zhang
Summary: In this study, a universal Cu(I) center was coupled with multiple strong visible-light-absorbing antennas to overcome the energy level limitations of current noble-metal complexes, resulting in the development of a broadband and strong visible-light-absorbing nonprecious complex. The systematic investigations demonstrated that this complex enables efficient intermolecular electron/energy transfer and exhibits outstanding performance for both energy- and electron-transfer reactions. These findings open up new possibilities for the development of efficient earth-abundant photosensitizers for boosting photosynthesis.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Materials Science, Multidisciplinary
Sihui Xiang, Changzhi Han, Chang Shu, Chong Zhang, Jia-Xing Jiang
Summary: Conjugated polymer photocatalysts with D-A structure were developed, and the band gap of the polymers can be tuned by adjusting the number of fused-thiophene rings. Increasing the number of thiophene rings extends the visible light absorption range. The optimized molecular structure facilitates efficient photocatalytic hydrogen and oxygen evolution.
SCIENCE CHINA-MATERIALS
(2022)
Article
Chemistry, Physical
Zhaolin Li, Hua Fang, Zupeng Chen, Weixin Zou, Chengxiao Zhao, Xiaofei Yang
Summary: In this study, novel triazine-based conjugated polymer photocatalysts were designed and synthesized by introducing electron-drawing 1,3,4-oxadiazole units, demonstrating excellent photocatalytic hydrogen production performance.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Daniel Costabel, Ratnadip De, Franz Jacobi, Jonas Eichhorn, Konrad Hotzel, Afshin Nabiyan, Christof Neumann, Andrey Turchanin, Stephan Kupfer, Felix H. H. Schacher, Sven Rau, Benjamin Dietzek-Ivansic, Kalina Peneva
Summary: In this study, two organic-metal photocatalysts, P-L (PtCl2 and PdCl(2)), were proposed. X-ray photoelectron spectroscopy showed that their binding energies match precisely the binding energies of the respective M-(bpy)-Cl-2 complexes. Cyclic voltammetry measurements of the complexes displayed additional reduction potentials upon metal insertion. Light-driven catalysis demonstrated that both compounds are catalytically active, with P-Pt outcompeting P-Pd with a TON of 186 over 48 h in the presence of ascorbic acid (P-Pd: 50). Time-resolved spectroscopy on P-L and P-Pt yields insights into the light-induced intramolecular processes, and the role of different excitation states in the catalytic process.
Article
Materials Science, Multidisciplinary
Yang Zhang, Ning Cao, Xiaoming Liu, Fengting He, Bin Zheng, Chaocheng Zhao, Yongqiang Wang
Summary: Pure g-C3N4 (PCN) prepared by traditional thermal condensation polymerization has low polymerization of heptazine ring chains and a large number of charge recombination centers, resulting in undesirable photocatalytic performance. By thermal treatment with ammonium oxalate monohydrate, highly dispersed porous g-C3N4 nanosheets were produced, and the integrity of their in-plane heptazine ring chains was successfully improved without introducing heteroatoms. The obtained samples exhibited acceptable stability and photocatalytic activity, with a hydrogen reduction rate 11.2 times higher than that of PCN in the absence of the Pt co-catalyst.
SCIENCE CHINA-MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Tomoya Oshikiri, Haruki Jo, Xu Shi, Hiroaki Misawa
Summary: This study utilized the concept of modal strong coupling between metal nanoparticles and a nanocavity to enhance the efficiency of hot-hole injection. The results showed that the hybrid modes of the modal strong coupling system promoted hot-hole injection and proton/water reduction by hot electrons over a broad wavelength range.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Nanoscience & Nanotechnology
Takafumi Enomoto, Yui Tsuji, Xiang Li, Aya M. Akimoto, Ryo Yoshida
Summary: Polymer micelles are potential materials for efficient catalysis in their unique nanospaces. However, the design of polymer micelle-based nanoreactors for dual photocatalysis, involving both a photocatalyst and another catalyst, is still limited due to the lack of molecular insight. In this study, we investigated the cooperation between a photocatalyst and a hydrogen evolution catalyst immobilized within the shell of polymer micelle-based nanoreactors. Our results suggest the existence of fluctuated and contacted pairs of the two catalysts within the nanoreactors, and the reaction rates were influenced by molecular crowding within the shell. This study provides a basis for developing efficient polymer micelle-based nanoreactors for dual photocatalysis.
ACS APPLIED NANO MATERIALS
(2023)
Article
Biochemistry & Molecular Biology
Emily H. Edwards, Jana Jelusic, Saikat Chakraborty, Kara L. Bren
Summary: A study has demonstrated that utilizing acetylated cobalt microperoxidase-11 as a catalyst, [Ru(bpy)(3)](2+) as a photosensitizer, and ascorbic acid as an electron donor can efficiently produce hydrogen from water in a visible light-driven reaction, with the highest efficiency achieved at neutral pH. The catalyst designed in this way shows longevity and outperforms traditional electrochemical systems.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Yoshinobu Kamakura, Chomponoot Suppaso, Issei Yamamoto, Ryusuke Mizuochi, Yusuke Asai, Teruki Motohashi, Daisuke Tanaka, Kazuhiko Maeda
Summary: Researchers report a tin-based metal-organic framework that can convert CO2 into formic acid with a record high quantum yield of 9.8%, without the need for additional photosensitizers or catalysts. This study highlights the potential of metal-organic frameworks in photocatalytic CO2 reduction using solar energy.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Koya Hojo, Shunta Nishioka, Yugo Miseki, Yoshinobu Kamakura, Takayoshi Oshima, Kazuhiro Sayama, Thomas E. Mallouk, Kazuhiko Maeda
Summary: A Dion-Jacobson phase calcium niobate was synthesized using both a flux method and solid-state reaction. Chemical exfoliation of the proton-exchanged niobate produced colloidal Ca2Nb3O10- nanosheets for dye-sensitized H-2 evolution, with flux-based nanosheets showing higher activity compared to those synthesized by solid-state reaction, particularly in water splitting systems. The improved H-2 evolution properties of the flux-derived nanosheets could be attributed to more efficient electron transfer pathways demonstrated by transient absorption spectroscopy.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Biochemistry & Molecular Biology
Emily H. H. Edwards, Jennifer M. M. Le, Alison A. A. Salamatian, Noelle L. L. Peluso, Linda Leone, Angela Lombardi, Kara L. L. Bren
Summary: This study reports a system for visible light-driven hydrogen production from water. The system utilizes a synthetic mini-enzyme as a catalyst, which shows advantages in terms of catalyst turnover rate and longevity compared to other cobalt porphyrins. This lays the groundwork for future research to tailor proton reduction chemistry and expand to new reactivity.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2022)
Article
Engineering, Chemical
Hengyu Liu, Fei Zhao, Shouli Ming, Yuchang Du, Jinsheng Zhao, Wei Zhang, Junhong Zhang
Summary: Regulating substitution position is a feasible method to design high-performance conjugated polymers or polymer heterojunctions as photocatalysts.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Physical
Jie Zhang, Jinyan Shi, Zhiwei Cui, Siqi Chu, Ying Wang, Zhigang Zou
Summary: By calcinating a mixture of melamine and high proportion of KOH, three types of defects were successfully introduced into heptazine polymer, adjusting its band structure and enhancing its response to visible light. Different defects introduce different defect levels within the bandgap, playing different roles in the photocatalytic process.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Yuepeng Wang, Guipeng Ji, Wenqiang Ye, Fengtao Zhang, Yiding Wang, Yanfei Zhao, Zhimin Liu
Summary: By utilizing density functional theory (DFT) analysis, a series of electron donor-acceptor (D-A) conjugated organic polymers were designed and synthesized. These polymers showed high efficiency in photocatalytic CO2 reduction under visible light irradiation. One of the polymers, derived from anthraquinone and triphenylamine, exhibited a high rate and selectivity in producing CO without the need for sacrificial reductants. The selectivity could be attributed to the intrinsic hydrophobicity of the photocatalyst.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Han Li, Oliver S. Wenger
Summary: Our study demonstrates the concept that single excitation of the two-electron reduced forms of perylene diimides (PDIs) with green photons can produce excited states with similar or greater reducing power than the shorter-lived excited states of PDI radical monoanions. By performing multi-electron reduction of a photocatalyst with a sacrificial reagent before irradiation with low-energy photons, we can generate highly reactive excited states for photocatalytic reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Qi-Fa Chen, Yao Xiao, Rong-Zhen Liao, Ming-Tian Zhang
Summary: In this study, a molecular trinuclear nickel (TNC-Ni) catalyst for water oxidation was reported. The catalyst exhibited high catalytic performance and stability under neutral conditions (pH 7). The cooperation among the three nickel sites was found to play a vital role in charge accumulation and O-O bond formation.
Article
Multidisciplinary Sciences
Zenghao Wang, Haotian Bai, Wen Yu, Zhiqiang Gao, Weijian Chen, Zhiwen Yang, Chuanwei Zhu, Yiming Huang, Fengting Lv, Shu Wang
Summary: Researchers have developed a living material composed of conjugated polymers and bacterial biofilm for lactate detection and cancer cell counting. This conductive material optimizes bioelectronic processes and allows wireless transfer of electrical signals to a portable smartphone for analysis.
Article
Chemistry, Multidisciplinary
Ning Yang, Yuetong Kang, Yujie Cong, Xiaoyu Wang, Chuang Yao, Shu Wang, Lidong Li
Summary: Based on hydrophobic dye-modified gold nanoclusters, a novel emulsion containing these nanoclusters has been developed. The emulsion is able to penetrate cell membranes through a physical mechanism, and exhibits multifluorescence tracing and efficient photothermal killing capabilities.
ADVANCED MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Wen Yu, Mariia V. Pavliuk, Aijie Liu, Yue Zeng, Shengpeng Xia, Yiming Huang, Haotian Bai, Fengting Lv, Haining Tian, Shu Wang
Summary: Organic semiconductor-microbial photosynthetic biohybrid systems have great potential in light-driven biosynthesis. This study presents a novel photosynthetic biohybrid system based on transmembrane electron transport, enabling efficient electron transfer from organic semiconductor to microorganisms, thus enhancing biosynthesis.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Jian Sun, Xiaoran Zhang, Xia Wang, Jinlei Peng, Gang Song, Yufei Di, Fude Feng, Shu Wang
Summary: This study designs a bio-friendly organic nitrite donor and demonstrates its antitumor effect through specific reactions with certain species. The results show that this method effectively inhibits tumor growth at the cellular level and has potential for precision cancer therapy.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Zenghao Wang, Hongrui Lin, Miaomiao Zhang, Wen Yu, Chuanwei Zhu, Pengcheng Wang, Yiming Huang, Fengting Lv, Haotian Bai, Shu Wang
Summary: Bioelectronics is an interdisciplinary field that combines electronics and biology. Organic semiconductors, particularly water-soluble conjugated polymers (WSCPs), have shown great potential in improving bioelectronic performance and regulating bioelectronic processes. This review summarizes the significant contributions of WSCPs in regulating bioelectronic processes and discusses the latest advances in their applications in biosynthetic systems, photosynthetic systems, biophotovoltaic systems, and bioelectronic devices.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Multidisciplinary
Hong-Tao Zhang, Yu-Hua Guo, Yao Xiao, Hao-Yi Du, Ming-Tian Zhang
Summary: We reported here the development of a heterobimetallic NiFe molecular platform to investigate the synergistic effect of NiFe in water oxidation catalysis. Compared to homonuclear bimetallic compounds (NiNi and FeFe), the NiFe complex exhibited significant catalytic activity in water oxidation. Mechanistic studies showed that this enhanced activity is attributed to the effective promotion of O-O bond formation by NiFe synergy. The formation of Ni-III(mu-O)Fe-IV=O intermediate is the key step for O-O bond formation through intramolecular oxyl-oxo coupling between bridged O radical and terminal Fe-IV=O moiety.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Han Li, Cui Wang, Felix Glaser, Narayan Sinha, Oliver S. Wenger
Summary: This study reports a new approach to achieve control over blue-to-UV upconversion by tethering a naphthalene unit to a cyclometalated iridium-(III) complex, providing a better option for photochemical applications. The bichromophore demonstrated a higher triplet energy and longer lifetime compared to the parent complex. The threshold for blue-to-UV upconversion to shift from quadratic to linear excitation power dependence was consistently lower with the bichromophore. Additionally, the bichromophore showed long-term stability under blue irradiation and successfully drove chemical reactions that normally require UV light.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Wen Yu, Yue Zeng, Zenghao Wang, Shengpeng Xia, Zhiwen Yang, Weijian Chen, Yiming Huang, Fengting Lv, Haotian Bai, Shu Wang
Summary: Developing artificial symbionts with modular design can enhance the production of functional polypeptides using CO2 and N2 as substrates. The strategy improves intracellular ATP and NADPH levels and increases the production of gamma-PGA. This approach also provides an innovative method for creating photosynthetic systems on demand.
Article
Nanoscience & Nanotechnology
Ge Zhang, Yuke Li, Qining Ke, Junchen Bai, Fushuai Luo, Jiacheng Zhang, Yanfen Ding, Juan Chen, Peng Liu, Shu Wang, Chong Gao, Mingshu Yang
Summary: In this study, a polymeric antibacterial agent was prepared using the melt grafting method. It was found that the resulting composite material showed high antibacterial activity against E. coli and S. aureus, and the antibacterial effect became more pronounced with the prolongation of chlorinated time.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Hong-Tao Zhang, Fei Xie, Yu-Hua Guo, Yao Xiao, Ming-Tian Zhang
Summary: We report the first nonheme CuFe oxygen reduction catalyst, which shows exceptional selectivity and turnover frequency in the reduction of oxygen to water. The collaborative efforts of copper and iron play a crucial role in achieving these outstanding catalytic properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Editorial Material
Nanoscience & Nanotechnology
Shu Wang, Chengmei Zhong, Jong Seung Kim, Linqi Shi
ACS APPLIED BIO MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Ruilian Qi, Fengting Lv, Yue Zeng, Qi Shen, Yiming Huang, Haotian Bai, Libing Liu, Shu Wang
Summary: To combat viral infectious diseases efficiently, it is crucial to develop broadly applicable countermeasures. Elaborating the relationship between antiviral agents and viruses can lead to the development of efficient antiviral systems. This study used conjugated polymer-based photodynamic therapy to inhibit RNA virus infections and assessed antiviral efficiency using a pseudotyped virus composed of SARS-CoV-2 envelope and luciferase RNA genome. Different cationic CPs showed varying photoinactivation effects, with PPV and PMNT exhibiting highly efficient photoinactivation derived from the complete degradation of spike proteins, nucleocapsid proteins, and nucleic acids of SARS-CoV-2.
NPG ASIA MATERIALS
(2023)
Article
Chemistry, Applied
Jing Shi, Yu-Hua Guo, Fei Xie, Ming -Tian Zhang, Hong-Tao Zhang
Summary: The process of water oxidation is a challenging task in the development of artificial photosynthetic systems. The use of redox-active ligands in conjunction with metals has been recognized as an effective approach for managing this process. However, the detailed mechanisms of how the electronic effect of these ligands affects the reactivity of the catalytic centers are still unclear. In this study, the electronic effect of a series of mononuclear Ru complexes with redox-active ligands was investigated, and it was found that the ligand-centered oxidation plays a crucial role in the water oxidation process. This study provides important insights into the role of redox-active ligands in controlling the water oxidation process.
CHINESE JOURNAL OF CATALYSIS
(2023)