Article
Energy & Fuels
Haojie Li, Zhen Yao, Yilin Zhu, Xuetao Wang
Summary: This study investigates the influence of solvent type and properties on catalytic hydrogen production from ammonia borane. The results show that both acid and alkali can improve the efficiency of hydrogen production. The alkaline solution enhances the hydrolysis of ammonia borane by activating the H-O bond of water molecules. The hydrogen production rate and yield are lower in alcohol solvents compared to water, possibly due to the different strength of the O-H bond in the alcohol molecules.
Article
Chemistry, Physical
Cheng Peng, Yi Zhang, Yong Wang, Wei Liu, Yonggang Yang
Summary: Density functional theory was used to investigate the mechanistic pathways of the bifunctional iron complex [Fe(DCPE)(PhNCH2)2] catalyzed AB dehydrogenation and polyaminoborane formation. The computational results suggest a favorable proton transfer pathway between the metal center and ligand, leading to a kinetically feasible transition state with low energy barrier. The subsequent polyaminoborane formation involves the generation of nucleophiles, with the NH2BH2 moiety, featuring a nitrogen lone pair, playing a crucial role in the chain polyaminoborane formation.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Review
Chemistry, Physical
Wenfeng Zhao, Hu Li, Heng Zhang, Song Yang, Anders Riisager
Summary: Ammonia borane (AB) is a promising material for hydrogen storage and has attracted much attention in reductive organic transformations. This review summarizes the recent progress of AB-mediated transfer hydrogenation reactions of various substrates and discusses the synthesis protocols, reaction parameters, product distribution, and reactivity. The mechanism involving the action mode of AB and structure-activity relationships are also discussed, and the challenges and opportunities for AB-enabled transfer hydrogenation reactions are highlighted.
GREEN ENERGY & ENVIRONMENT
(2023)
Article
Environmental Sciences
Yifeng Xu, Ying Gu, Lai Peng, Ning Wang, Shi Chen, Chuanzhou Liang, Yiwen Liu, Bing-Jie Ni
Summary: Although moving bed biofilm reactors (MBBRs) have shown excellent antibiotic removal potentials, the mechanisms underlying this process are still not well understood. This study investigated the removal of ciprofloxacin in an enriched nitrifying MBBR, revealing the significant contributions of biomass adsorption and microbial-induced biodegradation. The results showed that the presence of ammonium enhanced the biodegradation rate through ammonia oxidizing bacteria (AOB)-induced cometabolism, while heterotrophs played a minor role in ciprofloxacin biodegradation. The findings suggest the feasibility of nitrifying biofilm systems for efficient antibiotic removal from wastewater.
Article
Chemistry, Multidisciplinary
Qin Zhu, Shuoqi Zhang, Jing Ma, Jun Zhu, Shuhua Li, Guixiang Zeng
Summary: The transfer hydrogenation of azobenzene with ammonia borane mediated by pincer bismuth complex 1 was studied using density functional theory calculations. The study revealed an unusual metal-ligand cooperation mechanism involving the saturation/regeneration of the C=N functional group on the pincer ligand. The reaction proceeds through the hydrogenation of the C=N bond, followed by the conversion of 3(CN) to a Bi-H intermediate, and eventually results in the production of N,N'-diphenylhydrazine and regeneration of the catalyst. The substitution of the phenyl group with a tert-butyl group on the pincer ligand improves the catalyst's performance.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Engineering, Environmental
Li-Jun Zhou, Ping Han, Mengyue Zhao, Yaochun Yu, Dongyao Sun, Lijun Hou, Min Liu, Qiang Zhao, Xiufeng Tang, Uli Kluemper, Ji-Dong Gu, Yujie Men, Qinglong L. Wu
Summary: This study evaluated the biotransformation mechanisms of different ammonia-oxidizing microorganisms on lincomycin and three fluoro-quinolone antibiotics, finding that ammonia-oxidizing archaea showed the best biotransformation capability for these antibiotics.
Article
Chemistry, Multidisciplinary
Huizhen Li, Ruirui Wang, Jiaxin Kang, Shujun Li, Ai-Ju Zhou, Dong-xue Han, Hong-Yu Guan, Douglas J. Austin, Yanfeng Yue
Summary: A series of linear diborazanes were synthesized through a nucleophilic reaction, with crystal structure influenced by alkylamine and dihydrogen bonds. Different conformations were observed and stabilized by DHBs.
Article
Environmental Sciences
Weijie Xu, Jingyong Liu, Ziyi Ding, Jiawei Fu, Fatih Evrendilek, Wuming Xie, Yao He
Summary: This study characterized and verified the pyrolysis mechanisms and volatiles products of medical mask belts, mask faces, and infusion tubes. The results are important for the treatment of medical wastes.
SCIENCE OF THE TOTAL ENVIRONMENT
(2022)
Article
Chemistry, Multidisciplinary
Sisi Liu, Mengfan Wang, Haoqing Ji, Lifang Zhang, Jiajie Ni, Najun Li, Tao Qian, Chenglin Yan, Jianmei Lu
Summary: Photocatalytic nitrogen reduction reaction (PNRR) is a sustainable approach for ammonia synthesis. By combining porous framework materials with a novel solvent-in-gas system, the activity of PNRR can be significantly improved. This system-level strategy is also applicable in photocatalytic CO2 reduction, making it an important component of photosynthetic methodology.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Hao Ge, Yasutaka Kuwahara, Kazuki Kusu, Hiromi Yamashita
Summary: Utilizing degeneratively-doped metal oxide and precious metal hybrids with plasmonic absorption in the visible-light region allows for efficient utilization of solar light in photothermal catalysis. Among various morphologies of Pt/MoO3 hybrids, the nanosheet-structured Pt/HxMoO3-y(Sheet) catalyst demonstrated the best performance in the photothermal synergistic catalysis of the RWGS reaction, attributed to its high specific surface area, proportion of exposed surface atoms, and optical transparency. Additionally, the Pt/HxMoO3-y(Sheet) hybrid contained the largest amount of surface O vacancies and exhibited the strongest plasmonic absorption, leading to its highest catalytic activity among the investigated hybrid catalysts.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)
Article
Engineering, Environmental
Wei Zhang, Anna M. Alessi, Sonia Heaven, James P. J. Chong, Charles J. Banks
Summary: Transitions in microbial community structure in response to increasing ammonia concentrations were studied in mesophilic anaerobic digesters. The addition of trace elements, organic loading rates, and hydraulic retention times influenced metabolic routes and community structures. The study demonstrated a quantitative approach using 14C isotope analysis alongside sequencing data to understand methanogenic pathways and microbial populations.
Article
Chemistry, Multidisciplinary
Gabriel Lopez, Dominik Keiner, Mahdi Fasihi, Tuomas Koiranen, Christian Breyer
Summary: The global chemical industry is poised to become the largest consumer of fossil fuels, posing challenges to defossilize its production. New green carbon feedstocks like electricity-based methanol and biomass-based methanol need to be developed. Increased plastic recycling can also reduce the demand for primary feedstock. The study suggests that an e-chemical transition pathway may be the most economically competitive route to defossilize the chemical industry.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Engineering, Environmental
Federico Atzori, Francesco Barzagli, Alberto Varone, Giacomo Cao, Alessandro Concas
Summary: It is well known that CO2 capture and re-use is one of the main challenges to tackle global warming. Aqueous ammonia solutions have shown promising potential as sorbents for CO2 capture, offering higher absorption capacity, lower energy requirements, and greater resistance to degradation compared to conventional alkanolamines. This study investigates the chemical absorption of CO2 in aqueous NH3 solutions and proposes a mathematical model to quantify the capture efficiency dynamics and sorbent composition. The results validate the model's effectiveness in designing and optimizing the capture process, considering the effects of temperature and sorbent concentration.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Instruments & Instrumentation
Gennady Vishnyakov, Alexander Yurin, Vladimir Minaev, Alexander Golopolosov
Summary: We propose a method for measuring the refractive index (RI) and spectral characteristics of transparent triangular prisms using the minimum deviation technique. This method simultaneously measures the RI for three different wavelengths to determine the spectral dependence of RI. Our experimental results show that this method can achieve high-precision measurements of RI and determine the spectral characteristics with low measurement uncertainty.
Article
Energy & Fuels
Simion Dragan, Hannelore Lisei, Flavia-Maria Ilea, Alexandru-Constantin Bozonc, Ana-Maria Cormos
Summary: In this study, a comprehensive mathematical model is presented to address climate change through the process of carbon dioxide capture using ammonia aqueous solutions. The model is validated and shows strong correlation with experimental results. Scaling up the model to simulate industrial-scale ammonia-based absorption process reveals its potential utility for future applications, including process optimization and control techniques for mitigating drawbacks. The model's ability to effectively replicate system behavior under various conditions highlights its importance.
Article
Chemistry, Physical
Li Guan, Fengxue Tan, Yanan Liang, Xiaofang Xu, Shichuang Han, Jianxin Guo, Jianglong Wang, Zhiyong Zhang, Xu Li
Summary: This study investigated the electronic properties of n-type LaAlO3/SrTiO3 (LAO/STO) interfaces with LaO and AlO2 terminations using first-principles calculations. The effects of surface termination and point defects on the electronic structures and conductivity of interfaces were analyzed in detail, providing theoretical guidance for tuning the conductivity of perovskite heterostructures.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Zhenlian Chen, Bjoern Schwarz, Xianhui Zhang, Wenqiang Du, Lirong Zheng, Ailing Tian, Ying Zhang, Zhiyong Zhang, Xiao Cheng Zeng, Zhifeng Zhang, Liyuan Huai, Jinlei Wu, Helmut Ehrenberg, Deyu Wang, Jun Li
Summary: This study provides experimental evidence of peroxo species formed and confined in silicate cathodes at high voltage, while Co2+/Co3+ redox dominates at low voltage. These findings offer important insights for the rational design of high-energy-density cathodes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Ravindra B. Weerasooriya, Jonathan L. Gesiorski, Abdulaziz Alherz, Stefan Ilic, George N. Hargenrader, Charles B. Musgrave, Ksenija D. Glusac
Summary: Even with the discovery of an ideal hydride donor, the conversion of CO2 to formate still faces sluggish kinetics. This suggests that the conventional hydride transfer mechanism may not be suitable for solar conversion of CO2 to formate.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Qinfu Zhao, Lei Chen, Bingbing Suo, Zhiyong Zhang, Dan Deng, Bo Zhou, Haiyan Zhu, Qi Song
Summary: Inspired by alkaline metal borohydrides and organic-inorganic hybrid perovskite, a complex structure of (CH3NH3)BH4 with high hydrogen capacity is predicted. Through analysis of electronic structures, it is concluded that (CH3NH3)BH4 can be synthesized by a substitution reaction. The structural symmetries, elastic constants, and electronic properties of (CH3NH3)BH4 are investigated, showing strong elastic anisotropy and the influence of a planar dihydrogen bonding network on the dehydrogenation reaction. The proposed dehydrogenation process of (CH3NH3)BH4 via intermediate compounds suggests that it can decompose spontaneously, similar to ammonium borohydride.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Multidisciplinary
Nicholas R. Singstock, Jessica C. Ortiz-Rodriguez, Joseph T. Perryman, Christopher Sutton, Jesus M. Velazquez, Charles B. Musgrave
Summary: The Chevrel phase (CP) is a promising class of molybdenum chalcogenides, and a new machine-learned descriptor (H-delta) has been developed to rapidly and accurately assess CP stability. This approach successfully synthesized underexplored tellurides CPs and confirmed their preference for cation channel site occupation, showing potential for accelerating the discovery of synthesizable materials within a sparse class.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Polymer Science
Kangmin Kim, Jasmine Sinha, Jeffrey W. Stansbury, Charles B. Musgrave
Summary: A new visible DCPI was developed with superior photo- and dark-curing efficiencies, offering new application opportunities in RPP, especially in cases involving highly light attenuating resins, surfaces with irregular features, and production lines where continued dark-curing downstream of light activation enhances efficiencies.
Article
Chemistry, Physical
Samantha L. Millican, Jacob M. Clary, Charles B. Musgrave, Stephan Lany
Summary: This study investigates the redox mediating defect mechanism of solar thermochemical hydrogen production candidate material Hercynite using first-principles calculations. The results show the importance of defect interactions and suggest that oxygen defect entropy can positively influence the expansion of the thermodynamic window. This study is significant for guiding the discovery and design of suitable oxides.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Samantha L. Millican, Ann M. Deml, Meagan Papac, Andriy Zakutayev, Ryan O'Hayre, Aaron M. Holder, Charles B. Musgrave, Vladan Stevanovic
Summary: This paper presents a new method for accurately predicting defect concentrations in complex oxides, taking into account atomic and magnetic disorder as well as effects beyond the dilute defect limit. Using this method, the predicted defect concentrations are in good agreement with experimental values.
CHEMISTRY OF MATERIALS
(2022)
Article
Dentistry, Oral Surgery & Medicine
Kangmin Kim, Alexis Mascarenas, Charles B. Musgrave, Jeffrey W. Stansbury
Summary: The study demonstrates a spontaneous redox polymerization process at the adhesive-composite interface to improve bonding prior to composite photocure. By providing time for passive interfacial diffusion of benzoyl peroxide into the aromatic amine-containing composite, redox-initiated interfacial polymerization can occur, leading to a significant increase in micro-tensile bond strength between the adhesive and composite.
Article
Materials Science, Multidisciplinary
Sarah K. Bull, Theodore Champ, Sai Raj, Alan W. Weimer, Charles B. Musgrave
Summary: Density functional theory was used to screen refractory materials as high-temperature hydrogen permeation barriers. The study calculated activation energies and analyzed the properties of diffusing hydrogen atoms in the materials. Experimental evaluation confirmed the resistance of some nitride materials to nitrogen loss at high temperatures. This research provides theoretical support for effective hydrogen barriers at high temperatures.
JOURNAL OF NUCLEAR MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Zachary-L Bare, Ryan N. Morelock, Charles B. Musgrave
Summary: A high-throughput computational framework is used to identify novel multinary perovskite redox mediators, specifically Gd-containing perovskite oxide compositions that split water. The framework employs empirical approaches to evaluate material stabilities, electronic properties, and oxygen vacancy thermodynamics. By applying this computational scheme, 83 promising Gd-containing perovskite oxides are discovered, with three exhibiting catalytic activity in splitting water.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Physical
Ryan J. Morelock, Zachary J. L. Bare, Charles B. Musgrave
Summary: In this study, a parameterization framework based on the bond-valence method (BVM) was developed, which captures the relative stabilities computed by density functional theory (DFT) using the BVM global instability index (GII). The framework was tested against a dataset of 188 experimentally observed perovskite oxides and showed improved accuracy in identifying the ground state structures.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Multidisciplinary
Nicholas R. Singstock, Charles B. Musgrave
Summary: By simulating the nitrogen reduction reaction mechanism on Fe2Mo6S8, the reasons for its high activity and selectivity are revealed, and new principles for designing stable multinary electrocatalysts for other reactions are proposed.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Paige Brimley, Hussain Almajed, Yousef Alsunni, Abdulaziz W. Alherz, Zachary J. L. Bare, Wilson A. Smith, Charles B. Musgrave
Summary: This study uses Grand Canonical Density Functional Theory (GC-DFT) to model the electrochemical CO2 reduction process over metal-and nitrogen-doped graphene catalysts (MNCs) and includes the effects of the applied potential. The results predict effective catalysis of CO2R by Sc, Ti, Co, Cu, and Zn-N4Cs at moderate to large reducing potentials. The GC-DFT-computed density of states analysis demonstrates the critical role of adsorbed *CO2- anion in CO2R activation.
Article
Chemistry, Physical
Qinfu Zhao, Jianpeng Guo, Mengyu Su, Bingbing Suo, Haiyan Zhu, Bo Zhou, Zhiyong Zhang, Qi Song
Summary: This study considers the influence of attempt frequency on ionic conductivity, calculates the attempt frequencies of carrier migrations in Na3OBH4 and Na3OBr using density functional theory, and investigates the effect of substituting Br- with the [BH4](-) anion on the conductivity of sodium cations.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
