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55. Bioinspired spike-like double yolk–shell structured TiO2@ZnIn2S4for efficient photocatalytic CO2reductionElectronic supplementary information (ESI) available. See DOI: 10.1039/d1cy02079j

Author

She, Ping, Guan, Buyuan, Sheng, Jiyao, Qi, Yuanyuan, Qiao, Guanyu, Rui, Hongbang, Lu, Geyu, Qin, Jun-Sheng, and Rao, Heng

Abstract

Photocatalytic carbon dioxide (CO2) reduction (PCR) into syngas is one of the sustainable approaches for recycling CO2into value-added chemical feedstocks. However, the PCR efficiency is often limited by the insufficient light-harvesting and poor charge separation. Herein, we design a spike-like double yolk–shell structured TiO2@ZnIn2S4(D-Y-TiO2@ZnIn2S4) photocatalyst with superior PCR efficiency. The unique design not only integrates advantages of increasing active sites, surface areas and light-harvesting capacity induced by the hierarchical morphology, but also facilitates photo-induced charge separation based on the heterojunction of TiO2and ZnIn2S4. Owing to the combination of structural and compositional merits, the optimized D-Y-TiO2@ZnIn2S4photocatalyst shows superior PCR performance (325.29 μmol CO per g; 227.18 μmol H2per g) under visible light. In addition, the ratio of CO/H2can be tuned from 0.03 to 1.43 by changing the sacrificial hole capture condition. This work provides a prospective way to obtain efficient PCR photocatalysts.

Published
2022
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61. Exposed Equatorial Positions of Metal Centers via Sequential Ligand Elimination and Installation in MOFs

Author

Yuan, Shuai, primary, Zhang, Peng, additional, Zhang, Liangliang, additional, Garcia-Esparza, Angel T., additional, Sokaras, Dimosthenis, additional, Qin, Jun-Sheng, additional, Feng, Liang, additional, Day, Gregory S., additional, Chen, Wenmiao, additional, Drake, Hannah F., additional, Elumalai, Palani, additional, Madrahimov, Sherzod T., additional, Sun, Daofeng, additional, and Zhou, Hong-Cai, additional

Published
2018
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65. [Ti8Zr2O12(COO)(16)] Cluster : An Ideal Inorganic Building Unit for Photoactive Metal-Organic Frameworks

Author

Yuan, Shuai, Qin, Jun-Sheng, Xu, Hai-Qun, Su, Jie, Rossi, Daniel, Chen, Yuanping, Zhang, Liangliang, Lollar, Christina, Wang, Qi, Jiang, Hai-Long, Son, Dong Hee, Xu, Hongyi, Huang, Zhehao, Zou, Xiaodong, Zhou, Hong-Cai, Yuan, Shuai, Qin, Jun-Sheng, Xu, Hai-Qun, Su, Jie, Rossi, Daniel, Chen, Yuanping, Zhang, Liangliang, Lollar, Christina, Wang, Qi, Jiang, Hai-Long, Son, Dong Hee, Xu, Hongyi, Huang, Zhehao, Zou, Xiaodong, and Zhou, Hong-Cai

Abstract

Metal-organic frameworks (MOFs) based on Ti-oxo clusters (Ti-MOFs) represent a naturally self-assembled superlattice of TiO2 nanoparticles separated by designable organic linkers as antenna chromophores, epitomizing a promising platform for solar energy conversion. However, despite the vast, diverse, and well-developed Ti-cluster chemistry, only a scarce number of Ti-MOFs have been documented. The synthetic conditions of most Ti-based clusters are incompatible with those required for MOF crystallization, which has severely limited the development of Ti-MOFs. This challenge has been met herein by the discovery of the [Ti8Zr2O12(COO)(16)] cluster as a nearly ideal building unit for photoactive MOFs. A family of isoreticular photoactive MOFs were assembled, and their orbital alignments were fine-tuned by rational functionalization of organic linkers under computational guidance. These MOFs demonstrate high porosity, excellent chemical stability, tunable photoresponse, and good activity toward photocatalytic hydrogen evolution reactions. The discovery of the [Ti8Zr2O12(COO)(16)] cluster and the facile construction of photoactive MOFs from this cluster shall pave the way for the development of future Ti-MOF-based photocatalysts. GRAPHICS

Published
2018
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66. Retrosynthesis of multi-component metal−organic frameworks

Author

Yuan, Shuai, primary, Qin, Jun-Sheng, additional, Li, Jialuo, additional, Huang, Lan, additional, Feng, Liang, additional, Fang, Yu, additional, Lollar, Christina, additional, Pang, Jiandong, additional, Zhang, Liangliang, additional, Sun, Di, additional, Alsalme, Ali, additional, Cagin, Tahir, additional, and Zhou, Hong-Cai, additional

Published
2018
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68. [Ti8Zr2O12(COO)16] Cluster: An Ideal Inorganic Building Unit for Photoactive Metal–Organic Frameworks

Author

Yuan, Shuai, primary, Qin, Jun-Sheng, additional, Xu, Hai-Qun, additional, Su, Jie, additional, Rossi, Daniel, additional, Chen, Yuanping, additional, Zhang, Liangliang, additional, Lollar, Christina, additional, Wang, Qi, additional, Jiang, Hai-Long, additional, Son, Dong Hee, additional, Xu, Hongyi, additional, Huang, Zhehao, additional, Zou, Xiaodong, additional, and Zhou, Hong-Cai, additional

Published
2017
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71. Spatially Separated Bifunctional Cocatalysts Decorated on Hollow-Structured TiO2for Enhanced Photocatalytic Hydrogen Generation

Author

She, Ping, Rao, Heng, Guan, Buyuan, Qin, Jun-sheng, and Yu, Jihong

Abstract

Efficient charge separation can promote photocatalysis of semiconductors. Herein, a hollow-structured TiO2sphere decorated with spatially separated bifunctional cocatalysts was designed, which exhibited enhanced photocatalytic hydrogen generation. Ultrasmall-sized MOx(M = Pd, Co, Ni, or Cu) nanoparticles (NPs) were first introduced into a zeolite via confinement synthesis, and then, hollow TiO2was fabricated by using the zeolite as a sacrificial template forming MOx@TiO2. Finally, Pt NPs were decorated on the outer shell, giving rise to MOx@TiO2@Pt, in which the MOxNPs and Pt NPs acted as hole capturers and electron sinks, respectively. Thanks to the enhanced light harvesting of the hollow structure and improved charge separation induced by the smaller-sized cocatalysts as well as spatially separated bifunctional cocatalysts, the as-prepared PdOx@TiO2@Pt catalyst exhibited a superior photocatalytic hydrogen-generation property (0.45 mmol h–1). This work demonstrates the advantage of the spatially separated bifunctional cocatalysts in enhancing the photocatalytic properties of semiconductors.

Published
2020
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81. Stable Metal–Organic Frameworks with Group 4 Metals: Current Status and Trends

Author

Yuan, Shuai, Qin, Jun-Sheng, Lollar, Christina T., and Zhou, Hong-Cai

Abstract

Group 4 metal-based metal–organic frameworks (MIV-MOFs), including Ti-, Zr-, and Hf-based MOFs, are one of the most attractive classes of MOF materials owing to their superior chemical stability and structural tunability. Despite being a relatively new field, MIV-MOFs have attracted significant research attention in the past few years, leading to exciting advances in syntheses and applications. In this outlook, we start with a brief overview of the history and current status of MIV-MOFs, emphasizing the challenges encountered in their syntheses. The unique properties of MIV-MOFs are discussed, including their high chemical stability and strong tolerance toward defects. Particular emphasis is placed on defect engineering in Zr-MOFs which offers additional routes to tailor their functions. Photocatalysis of MIV-MOF is introduced as a representative example of their emerging applications. Finally, we conclude with the perspective of new opportunities in synthesis and defect engineering.

Published
2024
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82. 3D Chiral Microporous (10,3)-a Topology Metal–Organic Framework Containing Large Helical Channels

Author

Li, Mei-Na, Du, Dong-Ying, Yang, Guang-Sheng, Li, Shun-Li, Lan, Ya-Qian, Shao, Kui-Zhan, Qin, Jun-Sheng, and Su, Zhong-Min

Abstract

A new 3D chiral metal–organic framework [Co2(BTT)(OH)(H2O)5]·5CH3OH·6DMA (1) has been synthesized using an achiral tritopic bridging ligand, 1,3,5-tris(2H-tetrazol-5-yl)benzene (H3BTT). 1possesses a (10,3)-a net containing large helical channels of 17.43 Å and exhibits a high solvent-accessible volume (calculated 79%). The N2adsorption and magnetic properties for 1have been examined.

Published
2024
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83. Face-Sharing Archimedean Solids Stacking for the Construction of Mixed-Ligand Metal–Organic Frameworks

Author

Qiu, Yu-Chen, Yuan, Shuai, Li, Xiao-Xin, Du, Dong-Ying, Wang, Cong, Qin, Jun-Sheng, Drake, Hannah F., Lan, Ya-Qian, Jiang, Lei, and Zhou, Hong-Cai

Abstract

Reticular chemistry has been an important guiding principle for the design of metal–organic frameworks (MOFs). This approach utilizes discrete building units (molecules and clusters) that are connected through strong bonds into extended networks assisted by topological considerations. Although the simple design principle of connecting points and lines has proved successful, new design strategies are still needed to further explore the structures and functions of MOFs. Herein, we report the design and synthesis of two mixed-ligand MOFs, [(CH3)2NH2]4[Zn4O]4[Zn(TCPP)]5[BTB]8/3(PCN-137) and [Zr6(μ3-O)4(μ3-OH)4][TCPP][TBTB]8/3(PCN-138) (BTB = 1,3,5-benzene(tris)benzoate, TBTB = 4,4′,4″-(2,4,6-trimethylbenzene-1,3,5-triyl)tribenzoate, and TCPP = tetrakis(4-carboxyphenyl)porphyrin) by the stacking of face-sharing Archimedean solids. In these two MOFs, high-symmetrical metal clusters serve as vertices, and tritopic or tetratopic carboxylate ligands function as triangular and square faces, leading to the formation of two kinds of Archimedean solids (rhombicuboctahedron and cuboctahedron). Furthermore, the ordered accumulation of Archimedean solids successfully gives rise to 3D structures through face-sharing, highlighting the polyhedron-based approach for the design and preparation of MOFs. In addition, PCN-138 was utilized as a heterogeneous catalyst toward CO2photoreduction under visible-light irradiation. This structure shows high photocatalytic activity, which can be attributed to the coexistence of photosensitizing porphyrin fragments and Zr-oxo centers within the PCN-138 scaffold.

Published
2024
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84. [Ti8Zr2O12(COO)16] Cluster: An Ideal Inorganic Building Unit for Photoactive Metal–Organic Frameworks

Author

Yuan, Shuai, Qin, Jun-Sheng, Xu, Hai-Qun, Su, Jie, Rossi, Daniel, Chen, Yuanping, Zhang, Liangliang, Lollar, Christina, Wang, Qi, Jiang, Hai-Long, Son, Dong Hee, Xu, Hongyi, Huang, Zhehao, Zou, Xiaodong, and Zhou, Hong-Cai

Abstract

Metal–organic frameworks (MOFs) based on Ti-oxo clusters (Ti-MOFs) represent a naturally self-assembled superlattice of TiO2nanoparticles separated by designable organic linkers as antenna chromophores, epitomizing a promising platform for solar energy conversion. However, despite the vast, diverse, and well-developed Ti-cluster chemistry, only a scarce number of Ti-MOFs have been documented. The synthetic conditions of most Ti-based clusters are incompatible with those required for MOF crystallization, which has severely limited the development of Ti-MOFs. This challenge has been met herein by the discovery of the [Ti8Zr2O12(COO)16] cluster as a nearly ideal building unit for photoactive MOFs. A family of isoreticular photoactive MOFs were assembled, and their orbital alignments were fine-tuned by rational functionalization of organic linkers under computational guidance. These MOFs demonstrate high porosity, excellent chemical stability, tunable photoresponse, and good activity toward photocatalytic hydrogen evolution reactions. The discovery of the [Ti8Zr2O12(COO)16] cluster and the facile construction of photoactive MOFs from this cluster shall pave the way for the development of future Ti-MOF-based photocatalysts.

Published
2024
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89. A stable metal–organic framework with suitable pore sizes and rich uncoordinated nitrogen atoms on the internal surface of micropores for highly efficient CO2 capture

Author

Bao, Shao-Juan, primary, Krishna, Rajamani, additional, He, Ya-Bing, additional, Qin, Jun-Sheng, additional, Su, Zhong-Min, additional, Li, Shun-Li, additional, Xie, Wei, additional, Du, Dong-Ying, additional, He, Wen-Wen, additional, Zhang, Shu-Ran, additional, and Lan, Ya-Qian, additional

Published
2015
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