Review
Chemistry, Multidisciplinary
Ana Sousa-Castillo, Andrea Marino-Lopez, Begona Puertolas, Miguel A. Correa-Duarte
Summary: Bioorthogonal chemistry has provided a powerful tool for performing biocompatible chemospecific reactions in living systems, particularly in the areas of genetic encoding systems, bioimaging, and cancer therapy. This Minireview focuses on recent advances in the use of heterogeneous catalysts for bioorthogonal reactions, discussing the synthetic strategies of Pd-, Au-, and Cu-based materials, their applications in activating caged fluorophores and prodrugs, and the potential of using external stimuli for targeted drug release in diseased tissues. The review also highlights future directions and challenges in this emerging field.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Thermodynamics
Lili Ye, Dezhi Wang, Huiting Bian, Bei Li, Wei Gao, Mingshu Bi
Summary: The autoignition behavior of o-xylene at low temperatures is similar to alkanes. A detailed investigation of the chemical kinetics of oxygen additions with the o-xylyl radical was presented in this paper. The predicted oxygen addition kinetics explains the alkane-like autoignition behavior of o-xylene and the lower ignition reactivity due to the lower yield of QOOH, a key intermediate to chain branching.
COMBUSTION AND FLAME
(2021)
Article
Multidisciplinary Sciences
Wenhao Sun, Yonggang Xiang, Zhihui Jiang, Shengyao Wang, Nan Yang, Shangbin Jin, Linhao Sun, Huailong Teng, Hao Chen
Summary: Research on directed generation of ROSs induced by polymeric conjugation in nonmetallic conjugated microporous polymers (CMP) has been reported. The introduction of alkynyl groups allows for tunable molecular oxygen activation, affecting the directed generation of ROSs. The presence or absence of alkynyl bridges influences the mechanism of ROS generation in these CMPs.
Article
Chemistry, Physical
Olivia C. Williams, Carsten Sievers
Summary: Currently, there is no clear consensus on the active oxygen species in heterogeneous catalyzed hydrocarbon oxidation reactions, and more effective methods for characterization and quantification are needed. While several methods are effective for describing certain oxygen species, there is no method that comprehensively characterizes all active oxygen species. The most promising approach is oxygen isotope exchange coupled with infrared spectrometry and inline mass spectrometry.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Chemistry, Multidisciplinary
Michael D. Zott, Jonas C. Peters
Summary: This study details Fe-mediated AO electrocatalysis with a high TON and fast AO rate, highlighting the promising potential of Fe as a metal catalyst for further development in metal-mediated AO catalysis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Jiaxin Song, Kai Zhang, Zhongye Huang, Jinyu Zhao, Zhengyi Yang, Lingbo Zong, Jianbin Chen, Congxia Xie, Xiaofei Jia
Summary: A Pd/Cu bimetal-loaded porous organic polymer catalyst was prepared and used in the oxidation of alkynes with O2 as the oxidant to produce 1,2-diketones. The catalyst exhibited high surface areas, hierarchical porosity, and good thermal stability.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Review
Chemistry, Multidisciplinary
Sangyong Shin, Robert Haaring, Jungseob So, Yunji Choi, Hyunjoo Lee
Summary: Single-atom catalysts (SACs), single-atom alloys (SAAs), and ensemble catalysts are heterogeneous atomic catalysts with intentionally controlled surface metal atomic structures. These catalysts have received significant attention for their ability to fully utilize precious metals and induce unique surface reactions. However, durability and stability are crucial factors that need to be considered for practical applications. The properties of the support material and the susceptibility to impurities can significantly affect the performance of these catalysts. High durability heterogeneous atomic catalysts have great potential for sustainable chemical production.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Chemistry, Physical
Fanyu Wang, Yaqin Feng, Zhongsen Wang, Yi Liu, Huayu Gu, Xiao Liu
Summary: The researchers constructed and regulated the surface oxygen vacancies over epsilon-MnO2 with the aid of K doping to activate H2O, accelerating the reaction rate. The addition of K+ not only increased the adsorption sites for negatively charged oxygen atoms of HCHO but also provided oxygen vacancies to induce more active hydroxyl species from water activation. The K-doped epsilon-MnO2 catalyst showed efficient HCHO oxidation, removing 90% of HCHO at 74°C.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Li Zhao, Piaoping Yang, Song Shi, Guozhi Zhu, Xiao Feng, Weiqing Zheng, Dionisios G. Vlachos, Jie Xu
Summary: Activation of molecular oxygen for selective alcohol oxidation is achieved using a heterogeneous ligand method to prepare a high-efficiency vanadium carbon catalyst. Chemisorbed oxygen and pentavalent vanadium oxide are found to be crucial for catalyst performance. The V-C catalyst activates molecular oxygen to singlet oxygen or its analogue and carries out the reaction through C-H bond activation. The catalyst also shows high efficiency in selectively oxidizing hydroxyl groups in other substrates, providing guidance for the development of nonprecious metal catalysts for aerobic oxidation.
Article
Chemistry, Physical
Xinran Li, Indroneil Roy, Vidhya Chakrapani
Summary: A new design strategy for bifunctional electrocatalysts is proposed, doping the MnOx lattice with electropositive or electronegative elements to incorporate electron-rich donor and electron-poor acceptor defects. The BiMnOx catalyst shows promising OER/ORR activities comparable to state-of-the-art commercial Pt or RuO2 catalysts and exhibits stability for more than 3 hours of continuous polarization. This work provides a pathway for controlling electrocatalytic activities through tuning defects in perovskite-based oxides.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Qiyu Lian, Lingling Hu, Dingren Ma, Yimu Jiao, Dehua Xia, Yajing Huang, Zhuoyun Tang, Wei Qu, Huinan Zhao, Chun He, Daniel D. Gang
Summary: This study demonstrates that interstitial atomic Bi anchored in the lattice interstice of MnO2 can boost the catalytic oxidation reactions by triggering an alternative twofold O-2 activation, weakening the O-2 dissociation energy barrier by reconstructing the local charge landscape and elongating the O-O bond length.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Multidisciplinary Sciences
Yanyan Zhao, Sheng Dai, Ke R. Yang, Sufeng Cao, Kelly L. Materna, Hannah M. C. Lant, Li Cheng Kao, Xuefei Feng, Jinghua Guo, Gary W. Brudvig, Maria Flytzani-Stephanopoulos, Victor S. Batista, Xiaoqing Pan, Dunwei Wang
Summary: Atomically dispersed catalysts have shown high activity for selective oxidation of carbon monoxide with excess hydrogen, but their stability is not ideal. This study demonstrates that introducing a structural component to minimize the diffusion of the active metal center significantly improves stability without compromising activity. By using a dinuclear iridium heterogeneous catalyst as a study platform, two types of oxygen species, interfacial and bridge, are identified to work together for both activity and stability. This work provides important insights into the synergistic effect between the active metal center and the supporting substrate, with potential broad applications for atomically dispersed catalysts.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Multidisciplinary
Wenjuan Zhu, Akhilesh Kumar, Jin Xiong, Macon J. Abernathy, Xiao-Xi Li, Mi Sook Seo, Yong-Min Lee, Ritimukta Sarangi, Yisong Guo, Wonwoo Nam
Summary: The nature of reactive intermediates and the cis-dihydroxylation mechanism of arenes and olefins have been studied extensively in the past few decades. In this study, the reaction between a spectroscopically characterized mononuclear nonheme iron(III)-peroxo complex and olefins and naphthalene derivatives has been investigated. The results show that the nonheme iron(III)-peroxo complex is a nucleophile and reacts with olefins and naphthalenes to yield cis-diol products. This study presents the first example of cis-dihydroxylation of substrates by a nonheme iron(III)-peroxo complex.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Engineering, Environmental
Ruhua Zha, Yinghui Niu, Caiyun Liu, Liu He, Min Zhang
Summary: This study found that the BiVO4-Bi2S3 heterojunction constructed by oxygen vacancies can effectively catalyze the NO oxidation reaction, increase reaction efficiency by reducing the level of carrier recombination, and form active oxygen species through the exchange of adsorbed oxygen and lattice oxygen to efficiently remove NO.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Green & Sustainable Science & Technology
Yi Chen, Yuntong Dai, Yanwei Li, Zexi Hou, Baoyu Gao, Qinyan Yue, Qian Li
Summary: By using carboxymethyl chitosan hydrogel as a template, CuO nanoparticles wrapped into nitrogen-doped carbon nanocomposites (CuO@NCs) with abundant oxygen vacancies (OVs) were synthesized in one step. The obtained CuO@NCs showed excellent photothermal catalytic properties, achieving efficient activation of molecular oxygen under visible-light irradiation and effectively degrading bisphenol F (BPF) in complex aqueous environments and actual water matrices. Density functional theory (DFT) calculations revealed that the enhanced properties of OVs for molecular oxygen adsorption and the accelerated properties of graphitic N for electron transfer contributed significantly to the molecular oxygen activation and charge separation efficiency, resulting in a large amount of reactive oxygen species (ROS) generation.
JOURNAL OF CLEANER PRODUCTION
(2023)
Article
Chemistry, Applied
Pingping Wu, Haijun Liu, Yunxiang Cao, Shibo Xi, Zhiheng Li, Zhengke He, Lei Song, Jing Xu, Peng Bai, Lianming Zhao, Svetlana Mintova, Zifeng Yan
Summary: A series of MCF supported Au-Pt NP catalysts were designed in this study to reveal the essence, and an improved catalytic performance was observed on bimetallic catalyst, attributed to the geometric and electronic changes of active sites after formation of Au-Pt alloy NPs.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Chemistry, Physical
Chunzheng Wang, Ningkun Xu, Ting-Ting Liu, Weisong Xu, Hailing Guo, Yanpeng Li, Peng Bai, Xin-Ping Wu, Xue-Qing Gong, Xinmei Liu, Svetlana Mintova
Summary: This study reveals the impact of mechanical compression on Pd/NaY catalysts, which enhances the selectivity of the oxidative carbonylation of methanol to DMC by controlling the ratio of Pd species. The Pd clusters obtained under mechanical treatment show excellent catalytic performance, highlighting the importance of considering structural changes in metal-containing zeolite catalysts in heterogeneous catalysis.
JOURNAL OF CATALYSIS
(2021)
Article
Materials Science, Multidisciplinary
Youhe Wang, Tingting Li, Chencan Li, Jinzhi Lu, Chang Dai, Fazle Subhan, Peng Bai, Hongman Sun, Rui Feng, Zifeng Yan
Summary: The development of a sustainable synthesis route for Fe-ZSM-5 zeolites is important for their diverse applications. A novel dry gel conversion method was reported for one-pot synthesis of Fe-ZSM-5 zeolites, which does not require adding templates or seed crystals, improving synthesis efficiency and reducing environmental pollution. Characterization results showed that Fe-ZSM-5-In has enhanced acid amount and better distribution of framework Fe3+ species compared to Fe/ZSM-5-Im.
JOURNAL OF MATERIALS SCIENCE
(2021)
Article
Nanoscience & Nanotechnology
Pingping Wu, Zhengke He, Yonghui Liu, Lei Song, Chunzheng Wang, Edgar Muhumuza, Peng Bai, Lianming Zhao, Svetlana Mintova, Zifeng Yan
Summary: The study found that a modified catalyst consisting of nanosized Au-Pd particles with SnOx can enhance benzaldehyde selectivity by modulating the affinity of reactants and products on the catalyst surface through redox switching. Additionally, the presence of SnOx promotes improved catalytic activity.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Applied
Peng Bai, Miaomiao Yang, Xuejiao Chen, Yonghui Liu, Wei Yang, Lianming Zhao, Pingping Wu, Chunzheng Wang, Svetlana Mintova, Zifeng Yan
Summary: In this study, the VOX/Al2O3 catalyst was modified by boric acid, which significantly improved its stability and reduced coke deposition. The boron decreased the polymerization degree of VOX species, generating a high proportion of isolated vanadium species, thereby enhancing the stability of the catalyst. Boron interacted with Al and V, reducing the amounts of acid sites and alleviating coke deposition rate. The presence of boron promoted the desorption of propylene, improving the selectivity and stability of the catalyst.
Article
Chemistry, Applied
Peng Bai, Tao Zhou, Xiaohua Wang, Xiaofei Liu, Yi Wang, Yue Wang, Edgar Muhumuza, Yonghui Zhang, Pingping Wu
Summary: A series of Au-Pd alloy nanoparticles catalysts supported on gamma-Al2O3 were synthesized using MPTMS as an anchoring ligand. The results showed that the catalysts modified with MPTMS exhibited high catalytic activity and benzaldehyde selectivity, which can be attributed to the anchoring and dispersion effect of MPTMS on Au-Pd NPs and the formation of more surface Lewis acid sites.
Article
Chemistry, Applied
Yi Wang, Yonghui Zhang, Hongchao Fan, Pingping Wu, Meng Liu, Xinli Li, Jun Yang, Chaowei Liu, Peng Bai, Zifeng Yan
Summary: This study investigated the catalytic performance of four commercial zeolites (HZSM-5, H beta, HY, and SAPO-11) in the cracking of low-density polyethylene (LDPE) using a self-designed batch reactor. The acid strength of zeolites was found to be positively correlated with the cracking conversion. HZSM-5 and H beta zeolites exhibited high conversion rates, while large micropores promoted the formation of isomerized products but also led to significant coking. H beta zeolite achieved the highest yield of gasoline components, while HZSM-5 and HY showed high yields of aromatization products.
Article
Chemistry, Physical
Ke Huang, Ningkun Xu, Bin Liu, Peihua Zhang, Ge Yang, Hailing Guo, Peng Bai, Chunzheng Wang, Svetlana Mintova
Summary: Crystalline porous Mo-V-Bi oxides were prepared by hydrothermal synthesis, and the effects of organic additives on morphology and particle size were investigated. The 30 nm MoVBiO crystals showed high performance in the oxidation of methanol to methyl formate.
Article
Chemistry, Physical
Chunzheng Wang, Bin Liu, Panyue Liu, Ke Huang, Ningkun Xu, Hailing Guo, Peng Bai, Lixia Ling, Xinmei Liu, Svetlana Mintova
Summary: In this study, the reaction mechanism of methanol gas-phase indirect oxidative carbonylation for dimethyl carbonate (DMC) synthesis was investigated using a NaY zeolite catalyst doped with 1.0 wt% Pd. The reaction intermediates CO* and COOCH3* were identified and COOCH3* was determined as the rate-determining step. A Langmuir-Hinshelwood mechanism was proposed to explain the reaction process.
JOURNAL OF CATALYSIS
(2022)
Editorial Material
Chemistry, Applied
Zifeng Yan, Peng Bai, Svetlana Mintova, Feng-Shou Xiao, Bao-Lian Su
Article
Chemistry, Inorganic & Nuclear
Zhenxiang Zhao, Jun Yang, Ningkun Xu, Tian Nan, Pingping Wu, Chunzheng Wang, Xiaohua Wang, Peng Bai, Zifeng Yan, Svetlana Mintova
Summary: In this study, a highly dispersed In-Sn oxide catalyst with decreased OH groups and increased coordinatively unsaturated sites (CUS) was successfully prepared. The presence of water had no deleterious effect on the catalyst's activity due to the formation of water-tolerant Lewis acid sites (LAS). As a result, a record-high MLA yield of 57.6% was achieved using the In-Sn oxide catalyst. This work provides a new strategy for the design of non-zeolite metal oxide catalysts with improved water tolerance and high activity.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Lianming Zhao, Xiaonan Han, Yanfu Tong, Yanping Ding, Weichao Kong, Jiajun Wang, Bingyu Li, Jing Xu, Peng Bai, Xing Wei
Summary: In this study, we found that single metal atoms anchored on W2CO2 MXene can create efficient dual-active sites, thereby improving the efficiency of the anodic hydrogen oxidation reaction in alkaline exchange membrane fuel cells.
MATERIALS CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Bowen Liu, Peng Bai, Yang Wang, Zhun Dong, Pingping Wu, Svetlana Mintova, Zifeng Yan
Summary: In this study, the incorporation of TiO2 in the Ni/ZnO-Al2O3 adsorbent successfully inhibited the formation of inert spinel phase, improving the stability of the adsorbents and facilitating the adsorption of organo-sulfur compounds.
Article
Chemistry, Physical
Pingping Wu, Lei Song, Yue Wang, Xuehua Liu, Zhengke He, Peng Bai, Zifeng Yan
Summary: Enhancing benzaldehyde selectivity and improving oxygen transfer during the reaction can be achieved by generating more surface Lewis acid sites on ZrO2-modified alumina. The introduction of ZrO2 also enhances noble metal dispersion, leading to the formation of more active sites for improved catalytic activity.
APPLIED SURFACE SCIENCE
(2021)