Review
Chemistry, Multidisciplinary
Xuejiao Wu, Shunji Xie, Haikun Zhang, Qinghong Zhang, Bert F. Sels, Ye Wang
Summary: Transition metal sulfides are crucial semiconductors in the field of photocatalysis, playing a significant role in the conversion of lignocellulosic biomass into high-quality fuels and chemicals. Recent advancements in selective depolymerization of lignin and oxidative coupling of bioplatforms over metal sulfide semiconductors have been highlighted, emphasizing the importance of understanding reaction pathways and mechanisms for the rational design of efficient and selective photocatalysts.
ADVANCED MATERIALS
(2021)
Article
Polymer Science
Avinash Kumar Both, Deepa Choudhry, Chin Li Cheung
Summary: This paper introduces an environmentally friendly fabrication process for converting hemp fibers into biocomposites through a pectin-based crosslinking reaction. The water-based chemical approach utilizes pectin and lignin present in hemp fibers to crosslink and produce hemp fiber composites in one step. Compared to traditional processes, our green process uses water as the reaction solvent and operates at a mild temperature of 70°C, eliminating the need for petroleum-based organic solvents and high reaction temperatures. In addition, the study examines the effects of different mass ratios of pectin to hemp fiber and pH values on the compressive strength and bulk density of the hemp fiber composite materials, confirming the formation of ester bonds between pectin and lignin via transesterification.
JOURNAL OF APPLIED POLYMER SCIENCE
(2023)
Article
Engineering, Environmental
Shibo Shao, Ke Wang, Jason B. Love, Jialin Yu, Shangfeng Du, Zongyang Yue, Xianfeng Fan
Summary: A sulfur-rich zinc indium sulfide photocatalyst was developed to promote the cleavage of C-beta-O linkages in lignin, using water as a hydrogen donor. The reaction selectivity for aromatic monomers increased and the conversion rate of lignin model compounds improved significantly. This study provides a new and effective strategy to promote the cleavage of C-beta-O linkages and is helpful for the future development of photocatalytic lignin valorization.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Jayeeta Bhaumik, Yeddula Nikhileshwar Reddy, Seema Kirar, Neeraj Singh Thakur, Mahesh Daga Patil
Summary: A solar photocatalytic system based on porphyrin has been developed to directly depolymerize lignin and lignin-model compounds. The system's mechanism for lignin breakdown has been investigated and the catalyst's recovery and recyclability have been evaluated.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Biochemistry & Molecular Biology
Dingliang Dai, Jianhao Qiu, Guanglu Xia, Lu Zhang, Hong Ma, Luan Yang, Jianfeng Yao
Summary: Flower-like BiOI decorated with CdS nanodots and iodine vacancies (VI) was used as a photocatalyst for the valorization of sodium lignosulfonate (SLS) under visible light. The introduction of iodine vacancies adjusted the band configuration, enhanced light absorption, and acted as electron traps. The intimate contact between BiOI and CdS nanodots facilitated charge transfer, significantly improving the photocatalytic performance. The CdS/BiOI-VI heterostructure exhibited the highest yield of vanillin, surpassing other photocatalysts and showing great potential for lignin valorization.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2023)
Article
Chemistry, Multidisciplinary
Christopher W. J. Murnaghan, Nathan Skillen, Bronagh Hackett, Jack Lafferty, Peter K. J. Robertson, Gary N. Sheldrake
Summary: The valorization of biomass via photocatalysis is an expanding research field, but there is a need for further investigation into the impact of photocatalysis on recalcitrant compounds in biomass, such as lignin. Current research on lignin model compounds mainly focuses on the breakdown of small models with few linkages.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Xiaotong Xu, Shuqi Dai, Shuai Xu, Qi Zhu, Yuliang Li
Summary: In this study, a polymeric carbon nitride/polyhedral oligomeric silsesquioxane PDI heterojunction photocatalyst was prepared to overcome the charge localization effect and strong intermolecular aggregation in PDI, leading to improved cleavage conversion efficiency and promising application prospects.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Guannan Shen, Xinchuan Yuan, Yin Cheng, Sitong Chen, Zhaoxian Xu, Mingjie Jin
Summary: A novel pretreatment technology, DLCA, integrated with deep eutectic solvents (DESs) was used for lignocellulose fractionation and valorization. Low DES dosage and high fractionation efficiency were achieved, with high delignification ratio and cellulose preservation. The DLCA(DES) pretreatment showed superior bioconversion efficiency even at high solid loadings.
Review
Biochemistry & Molecular Biology
Cecilia Scimmi, Luca Sancineto, Jozef Drabowicz, Claudio Santi
Summary: This article provides a detailed overview of oxidative depolymerization of lignin and biomass valorization. It compares the advantages and disadvantages of different methods, highlights the green aspects, and gives an overview of selenium catalyzed lignin valorization.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Multidisciplinary Sciences
Tao Peng, Wenbin Zhang, Baiyao Liang, Guanwu Lian, Yun Zhang, Wei Zhao
Summary: This study reports a flow-cell system equipped with a highly-electrolyte permeable Rh diffusion electrode for electrocatalytic hydrogenation of important bio-oil aromatic molecules at industrial-scale current densities. The research shows that the high faradaic efficiencies and productivities can be achieved by using highly-electrolyte permeable Rh diffusion electrodes, which improves the industrial-scale productivity of the reaction.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Multidisciplinary
Yong Guo, Yaxuan Jing, Qineng Xia, Yanqin Wang
Summary: The escalating energy demand, depletion of fossil fuels, and abnormal climate change are considered important challenges in the 21st century. Using biomass and plastic as alternatives to fossil fuels is seen as a promising solution to create a carbon-neutral, waste-free society. Catalysis plays a crucial role in energy transformations, particularly in the cleavage of C-O and C-C bonds for producing chemicals and fuels. NbOx-based catalysts have shown exceptional ability in activating these bonds, making them important for biomass valorization and plastic upcycling. This work highlights the significance of understanding the activation of C-O and C-C bonds by NbOx-based catalysts and provides insights into future recommendations in this field.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Agricultural Engineering
Chao Liu, Bingyang Liu, Xing Wang, Zhanghong Xie, Lili Tong, Xiangchen Kong, Yuyang Fan, Rui Xiao
Summary: A tandem strategy combining photocatalytic preoxidation and ultrasonic cavitation depolymerization was proposed for lignin utilization, which greatly enhanced the depolymerization efficiency and product yield, providing a new idea for lignin valorization.
BIORESOURCE TECHNOLOGY
(2022)
Article
Multidisciplinary Sciences
Alexander Ahrens, Andreas Bonde, Hongwei Sun, Nina Kolln Wittig, Hans Christian D. Hammershoj, Gabriel Martins Ferreira Batista, Andreas Sommerfeldt, Simon Frolich, Henrik Birkedal, Troels Skrydstrup
Summary: Fibre-reinforced epoxy composites are widely used in load-bearing applications due to their light weight and high durability. However, the lack of viable recycling strategies for these composites has led to their disposal in landfills. This study presents a chemical recycling approach that allows for the recovery of polymer building blocks and intact fibres from epoxy composites.
Article
Green & Sustainable Science & Technology
Karelle S. Guiao, Arvind Gupta, Costas Tzoganakis, Tizazu H. Mekonnen
Summary: The effective utilization of biomass components is of great importance in the fields of energy and materials. Green processes, such as extrusion and reactive extrusion, are desired for their high yield and low cost. Reactive extrusion, with its combination of physical and chemical deconstruction, has shown promising results in the deconstruction of biomasses and recovery of valuable components.
JOURNAL OF CLEANER PRODUCTION
(2022)
Article
Chemistry, Multidisciplinary
Jinyuan Cheng, Xuze Liu, Chen Huang, Yunni Zhan, Caoxing Huang, Tingjun Chen, Xianzhi Meng, Chang Geun Yoo, Guigan Fang, Arthur J. Ragauskas
Summary: A biphasic solvent process combining deep eutectic solvents (DESs) and γ-valerolactone (GVL) was studied for efficient glucan saccharification, furfural production, and lignin recovery. This process significantly enhanced cellulose enzymatic saccharification by removing lignin and xylan, while preserving the structure of recovered lignin and achieving satisfactory furfural yield.
Article
Chemistry, Multidisciplinary
Sizhuo Yang, Daniel Streater, Christian Fiankor, Jian Zhang, Jier Huang
Summary: 2D covalent organic frameworks (COFs) have emerged as a promising class of organic luminescent materials due to their structural diversity. This study reports two highly emissive sp(2)-C-COFs and explores the correlation between structure and light absorption/emission, charge transfer (CT), and exciton dynamics. The research shows that the planarity, conjugation, orientation of the dipole moment, and interlayer aggregation play important roles in determining the light-harvesting ability and photoluminescent quantum yield of COFs.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Review
Chemistry, Inorganic & Nuclear
Thilini K. Ekanayaka, Guanhua Hao, Aaron Mosey, Ashley S. Dale, Xuanyuan Jiang, Andrew J. Yost, Keshab R. Sapkota, George T. Wang, Jian Zhang, Alpha T. N'Diaye, Andrew Marshall, Ruihua Cheng, Azad Naeemi, Xiaoshan Xu, Peter A. Dowben
Summary: Molecular multiferroic devices have the potential to become low-cost solid-state memory, but there are still challenges to overcome, including the issue of practical value.
Correction
Chemistry, Multidisciplinary
Sizhuo Yang, Daniel Streater, Christian Fiankor, Jian Zhang, Jier Huang
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Multidisciplinary Sciences
Ziman Chen, Dong Yan, Liang Ma, Yahui Zhang, Jingyan Zhang, Hui Li, Rebecca Khoo, Jian Zhang, Frantisek Svec, Yongqin Lv, Tianwei Tan
Summary: The study synthesized specific MOFs with reactive double bonds and successfully carried out copolymerization, enhancing the interfacial adhesion between MOFs and polymers. This led to the preparation of mixed matrix membranes capable of efficiently separating CO2, providing a new approach to saving energy and addressing environmental issues.
Article
Chemistry, Multidisciplinary
Li Ma, Yi Xie, Rebecca Shu Hui Khoo, Hadi Arman, Bin Wang, Wei Zhou, Jian Zhang, Rui-Biao Lin, Banglin Chen
Summary: In this study, an adaptive hydrogen-bonded organic framework was reported, which can selectively recognize and separate p-xylene. The single crystal structure and NMR studies demonstrated the efficient separation of xylene isomers by the organic framework.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Physical
Tiantian Feng, Daniel Streater, Bing Sun, Korlan Duisenova, Dong Wang, Yi Liu, Jier Huang, Jian Zhang
Summary: In this study, the photophysical properties of three highly crystalline imine-linked 2D COFs were systematically investigated using experimental and computational methods. It was found that the different electron affinities in the materials can influence the excited state, charge transfer direction, and lifetime, thus affecting the performance of the materials. One of the materials exhibited a greater degree of delocalization, resulting in a long-lived charge-separated state.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Christian Fiankor, James Nyakuchena, Rebecca Shu Hui Khoo, Xu Zhang, Yuchen Hu, Sizhuo Yang, Jier Huang, Jian Zhang
Summary: This study presents the design and synthesis of a highly porous and photoactive mixed-ligand MOF, showcasing the potential of MOFs as an ideal platform for studying energy transfer processes and the possibility of directly utilizing EnT processes in photocatalytic applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Inorganic & Nuclear
Guanhua Hao, Alpha T. N'Diaye, Thilini K. Ekanayaka, Ashley S. Dale, Xuanyuan Jiang, Esha Mishra, Corbyn Mellinger, Saeed Yazdani, John W. Freeland, Jian Zhang, Ruihua Cheng, Xiaoshan Xu, Peter A. Dowben
Summary: The X-ray-induced spin crossover transition of an Fe (II) molecular thin film was studied with and without a magnetic field. The thermal activation energy barrier for this transition was found to decrease in the presence of a magnetic field, leading to deviations from the expected spin state transition behavior. Additionally, the orbital moment was observed to decrease with increasing temperature relative to the spin moment near room temperature.
Article
Physics, Condensed Matter
Guanhua Hao, Ashley S. Dale, Alpha T. N'Diaye, Rajesh Chopdekar, Roland J. Koch, Xuanyuan Jiang, Corbyn Mellinger, Jian Zhang, Ruihua Cheng, Xiaoshan Xu, Peter A. Dowben
Summary: Compact domain features were observed in spin crossover [Fe{H2B(pz)(2)}(2)(bipy)] molecular thin film systems. Monte Carlo simulations support the presence of intermolecular interactions that can be described by a two-dimensional Ising model. These interactions contribute to the formation of largely high spin state domain structure.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2022)
Article
Chemistry, Multidisciplinary
Sizhuo Yang, Chongqing Yang, Chaochao Dun, Haiyan Mao, Rebecca Shu Hui Khoo, Liana M. Klivansky, Jeffrey A. Reimer, Jeffrey J. Urban, Jian Zhang, Yi Liu
Summary: Covalent organic frameworks (COFs) have shown great potential for various advanced applications due to their unique structure. Researchers have developed a synthetic approach that introduces nitrogen-containing heterocycles into COFs, leading to the introduction of new functionalities. This general strategy opens up possibilities for a broader range of functional porous crystalline materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Nanoscience & Nanotechnology
Yuchen Hu, Rebecca Shu Hui Khoo, Jingzhi Lu, Xu Zhang, Jian Zhang
Summary: Rare-earth metal-organic frameworks (RE-MOFs) are an attractive platform for constructing luminescent materials. This study successfully designed and synthesized a series of RE-MOFs with excellent thermal and chemical stability by incorporating a bulky tert-butyl group on a new carbazole-based ligand. These materials not only exhibit tunable emission but also demonstrate excellent thermal and DMF sensing capability.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Physics, Condensed Matter
Saeed Yazdani, Kourtney Collier, Grace Yang, Jared Phillips, Ashley Dale, Aaron Mosey, Samuel Grocki, Jian Zhang, Anne E. Shanahan, Ruihua Cheng, Peter A. Dowben
Summary: Using optical characterization, the study shows that the spin state of the spin crossover molecular complex [Fe{H2B(pz)(2)}(2)(bipy)] is influenced by the electric polarization of the adjacent polymer ferroelectric polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) thin film. The role of the PVDF-HFP thin film is significant but complex. UV-Vis spectroscopy measurements reveal that the electronic structure of [Fe{H2B(pz)(2)}(2)(bipy)] molecules in bilayers of PVDF-HFP/[Fe{H2B(pz)(2)}(2)(bipy)] can switch as a function of ferroelectric polarization at room temperature. The retention of voltage-controlled nonvolatile changes to the electronic structure in bilayers of PVDF-HFP/[Fe{H2B(pz)(2)}(2)(bipy)] strongly depends on the thickness of the PVDF-HFP layer. The PVDF-HFP/[Fe{H2B(pz)(2)}(2)(bipy)] interface may affect PVDF-HFP ferroelectric polarization retention in the thin film limit.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2023)
Article
Chemistry, Multidisciplinary
Yuchen Hu, Xin Zhang, Rebecca Shu Hui Khoo, Christian Fiankor, Xu Zhang, Jian Zhang
Summary: By reducing the size of the primary ligand, we synthesized NPF-320, a Zr-MOF with optimized pocket sizes. This MOF allows for the post-synthetic installation of three secondary linkers in all six permuted sequences, forming a quinary MTV-MOF. With the functionalization of these linkers, we can construct MTV-MOFs with variable porosity and unprecedented complexity and encoded synthetic sequence information.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Materials Science, Multidisciplinary
Ashley S. Dale, Saeed Yazdani, Thilini K. Ekanayaka, Esha Mishra, Yuchen Hu, Peter A. Dowben, John W. Freeland, Jian Zhang, Ruihua Cheng
Summary: In this work, clear evidence of magnetic anisotropy in the local orbital moment of a molecular thin film based on the SCO complex [Fe(H2B(pz)(2))(bipy)] (pz = pyrazol-1-yl, bipy = 2,2'-bipyridine) is provided. The magnetic easy axis for the orbital moment is found to be along the surface normal direction, indicating the presence of an anisotropic energy barrier in the high-spin state. The observed magnetocrystalline anisotropy is mostly due to spin-orbit coupling, with spin- and orbital-component anisotropies determined to be 30.9 and 5.04 meV molecule(-1), respectively. The g factor in the range of 2.2-2.45 is consistent with the expected values. This work paves the way for understanding the spin-state-switching mechanism in the presence of magnetic perturbations.
JOURNAL OF PHYSICS-MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Yuchen Hu, Rebecca Shu Hui Khoo, Jingzhi Lu, Xu Zhang, Jian Zhang
Summary: Rare-earth metal-organic frameworks (RE-MOFs) are a promising platform for constructing luminescent materials. The designed RE-MOFs in this study showed excellent thermal and chemical stability, making them potential candidates for applications in white-light emission and temperature-DMF sensing.
ACS APPLIED MATERIALS & INTERFACES
(2022)