Article
Chemistry, Multidisciplinary
Tongtong Jia, Di Meng, Ran Duan, Hongwei Ji, Hua Sheng, Chuncheng Chen, Jikun Li, Wenjing Song, Jincai Zhao
Summary: Prospects in light-driven water activation have led to rapid progress in hydrogenation reactions. In this study, a Ni2+-N-4 site built on carbon nitride was used for catalyzing the semihydrogenation of alkynes with water providing protons, powered by visible-light irradiation. Importantly, this photocatalytic approach enabled the production of diverse deuterated alkenes in D2O with excellent deuterium incorporation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yang Zhu, Wenyu Wang, Peng Gong, Yafei Zhao, Yuanbo Pan, Jianhua Zou, Rujiang Ao, Jun Wang, Huilan Cai, Hongwei Huang, Meili Yu, Huijuan Wang, Lisen Lin, Xiaoyuan Chen, Yuen Wu
Summary: As a rising generation of nanozymes, single atom enzymes show promise for cancer therapy due to their maximum atom utilization efficiency and well-defined electronic structures. This study develops an anion exchange strategy to produce a heteroatom-doped single atom enzyme with precise control, specifically sulfur (S)-and nitrogen (N)-decorated nickel single atom enzyme (S-N/Ni PSAE). The sulfurized S-N/Ni PSAE exhibits enhanced peroxidase-like and glutathione oxidase-like activities, triggering ferroptosis of tumor cells more effectively in vitro and in vivo compared to nitrogen-monodoped N/Ni PSAE.
Article
Nanoscience & Nanotechnology
Jun Wang, Qing Kuang, Xiaofang Su, Xiaowen Lu, Leipeng Leng, Mingyang Zhang, Chunmu Guo, Tong Li, Qian Xu, Shuhui Sun, J. Hugh Horton, Wei Wu, Zhijun Li
Summary: Supported single-atom catalysts are at the forefront of heterogeneous catalysis, with physicochemical properties that are highly interesting. This study demonstrates an efficient postsynthesis method for constructing singly dispersed palladium atoms on SAPO-31, showing promising application prospects in the semihydrogenation of alkynes. The catalyst exhibited outstanding performance in the semihydrogenation of phenylacetylene and 1-chloro-4-ethynylbenzene, as well as high activity in triethoxysilane oxidation, with retention of atomic dispersion and catalytic activity at high temperatures.
ACS APPLIED NANO MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Leilei Yin, Shuai Zhang, Mingzi Sun, Siyuan Wang, Bolong Huang, Yaping Du
Summary: This study reports cerium single atoms (Ce SAs) supported on a P, S, and N co-doped hollow carbon substrate (Ce SAs/PSNC) for the oxygen reduction reaction (ORR). The Ce SAs/PSNC exhibits excellent ORR stability and outperforms commercial Pt/C and most recent SACs. Ce SAs/PSNC-based liquid zinc-air batteries (ZABs) show a high and stable open-circuit voltage and a maximum power density. Theoretical calculations reveal that the introduction of S and P sites significantly modulate the electronic properties of Ce SA active sites, promoting the electroactivity of Ce SAs within the Ce SAs/PSNC.
ADVANCED MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Jianli Wang, Wei-Qiang Han
Summary: Lithium sulfur batteries, with high theoretical capacity and energy density, face challenges such as poor conductivity of active sulfur, large volume expansion of cathode, and shuttle effect of lithium polysulfides. Heteroatom doping is proposed to manipulate the electronic structure and improve the performance of sulfur host materials for enhanced cell performance.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Review
Materials Science, Ceramics
M. Atikur Rahman
Summary: BaTiO3(BT) is a crucial ceramic material in the semiconductor market due to its multifunctional properties. Doping techniques have received considerable attention to enhance the attractive qualities of BaTiO3 and broaden its applications in modern technologies. The choice of synthesis method and doping components is crucial for producing high purity and suitable grain size BaTiO3 particles for desired applications. This review aims to increase understanding of doping sites and possible applications based on previous literature.
JOURNAL OF ASIAN CERAMIC SOCIETIES
(2023)
Article
Chemistry, Applied
Yue Shao, Zhengtai Zha, Hong Wang
Summary: Electrocatalysts play a crucial role in the development of renewable energy technologies, with heteroatom-doped porous carbon-supported single-atom electrocatalysts showing promising advantages. Rapid advancements have been made in recent years in the synthesis, characterization, and performance enhancement of SAC-HDPCs through advanced characterization techniques and innovative synthetic strategies.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Physical
Gianvito Vile, Giovanni Di Liberto, Sergio Tosoni, Alessandra Sivo, Vincenzo Ruta, Maarten Nachtegaal, Adam H. Clark, Stefano Agnoli, Yajun Zou, Aleksandr Savateev, Markus Antonietti, Gianfranco Pacchioni
Summary: This study reports the high catalytic performance of a family of Cu-based single-atom catalysts for triazole synthesis. The use of a carbon nitride carrier as a ligand for atomically dispersed copper species improves the catalyst activity and selectivity.
Review
Chemistry, Multidisciplinary
Man Yixiao, Zhao Jinyu, Liu Shipeng, Pan Qingyan, Zhao Yingjie
Summary: Graphdiyne (GDY) as a new carbon allotrope with unique 2D structure and semiconductor characteristics, has extensive practical application prospects in energy, catalysis, and other fields. Considerable efforts have been made in recent years to develop doped GDY materials, which can further tune their structure and properties for expanded applications. This review provides a comprehensive overview of heteroatom doped GDYs, including synthesis, structures, properties, applications in nanotechnology, and future prospects.
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
(2021)
Article
Chemistry, Physical
Chaofeng Zhu, Yang Wang, Jiawei Xue
Summary: A K+-doped and cyanamide defects modified carbon nitride (CCNK) with free-standing nanosheets in water was synthesized using a bottom-up self-exfoliated strategy. The cyanamide moiety and K+ in the framework play a crucial role in enhancing hydrophilicity and efficiently suppressing electron-hole pair recombination. CCNK exhibits impressive photocatalytic hydrogen evolution activity (132.6 µmol h(-1)), which is 22 times higher than bulk carbon nitride (6.0 µmol h(-1)), surpassing other carbon nitride-based photocatalysts. This work provides a innovative facile self-exfoliated strategy for the preparation of ultrathin carbon nitride nanosheets and paves the way for high-performance photocatalysts using carbon nitride-based powders.
Review
Chemistry, Multidisciplinary
Min Ji Im, Jin Il Kim, Seok-Ki Hyeong, Byung Joon Moon, Sukang Bae
Summary: Graphene quantum dots (GQDs) are zero-dimensional carbon-based materials with exceptional optical, electrical, and optoelectrical properties. Their unique electronic band structures, influenced by quantum confinement and edge effects, differentiate GQDs from other carbon nanostructures. Various methods for synthesizing functionalized GQDs using different doping routes are comprehensively reviewed in this article, and the current challenges and future directions for GQDs research are discussed in detail based on previous reports.
Article
Chemistry, Physical
Sitan Li, Bo Feng, Xiaoxin Zhang, Jing Tian, Dan Wang, Yan Pei, Minghua Qiao, Yefei Li, Baoning Zong
Summary: A K, S, and O co-doped PCN (akut-CN) was successfully synthesized through one-pot polymerization of urea and thiourea in the presence of KCl and NaOH, which exhibited an unprecedentedly high H2O2 production rate of 4.46 mM h-1 under visible light irradiation, about 210 times that of undoped PCN. The heteroatom doping and the incorporation of cyano and hydroxyl groups into akut-CN were found to enhance light absorption, facilitate the separation and transfer of photogenerated charges, and improve the surface electronegativity and the O2 adsorption capacity and strength, thereby boosting the reaction kinetics. This work highlights the great potential of elaborately decorated PCN in photocatalytic O2 reduction to H2O2 and paves the way for decentralized production and application of H2O2.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Hong Bao, Liang Wang, Gao Li, Li Zhou, Yun Xu, Zheng Liu, Minghong Wu
Summary: In this study, boron-doped carbon nitride nanotubes were designed and prepared, which significantly increased their specific surface area, active sites, graphitization degree, and hindered the recombination of photogenerated electron-hole pairs. Moreover, the boron-doped carbon nitride nanotubes exhibited a longer fluorescence lifetime and higher hydrogen evolution rate compared to tubular carbon nitride.
Article
Chemistry, Physical
Ji-Kai Sun, Yu-Wei Pan, Meng-Qian Xu, Lei Sun, Shaolong Zhang, Wei-Qiao Deng, Dong Zhai
Summary: Replacing fossil fuels with fuel cells is a feasible solution to reduce global energy shortages and environmental pollution. Catalysts with high catalytic activity of oxygen reduction reaction (ORR) are significant for the development of fuel cells. This study explored Pt single-atom catalysts (SACs) supported on heteroatom-doped graphene for ORR and identified Pt-C-4 and Pt-C3O1 structures with low overpotential. It was found that B doping weakens Pt's adsorption capacity, while N or O doping enhances it, which was verified on Fe SACs. The electronic interaction analysis and the proposed descriptor, corrected d-band center (e(d-corr)), explained the mechanism and provided a regulatory strategy for ORR catalyst design.
Article
Engineering, Environmental
Jinwei Bai, Rui-Ting Gao, Nhat Truong Nguyen, Xianhu Liu, Xueyuan Zhang, Lei Wang
Summary: A heterogeneous doping approach, combining surface gradient doping with bulk doping, can enhance charge carrier transport and improve selectivity for H2O2 production in photoelectrochemical (PEC) water splitting. By inducing gradient Nb and homogeneous Mo doping into the BiVO4 photoanode, charge separation and carrier transfer are promoted, leading to high selectivity for H2O2 generation and suppress ion of O2 production.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Erik Kirstein, Evgeny A. . Zhukov, Dmitri R. . Yakovlev, Nataliia E. Kopteva, Carolin Harkort, Dennis Kudlacik, Oleh Hordiichuk, Maksym V. Kovalenko, Manfred Bayer
Summary: This research investigates the coherent spin dynamics of Ruddlesden-Popper (PEA)2PbI4 perovskites through picosecond pump-probe Kerr rotation experiments in an external magnetic field. The study identifies the Larmor spin precession of resident electrons with a spin dephasing time of 190 ps, as well as a long longitudinal spin relaxation time of 25 μs in weak magnetic fields. A significant anisotropy of the electron g-factor is also found, with in-plane value of +2.45 and out-of-plane value of +2.05. Furthermore, the exciton out-of-plane g-factor is measured to be +1.6 using magneto-reflectivity. This work contributes to the understanding of the spin-dependent properties and spin dynamics of two-dimensional perovskites.
Article
Chemistry, Multidisciplinary
Federico Montanarella, Quinten A. Akkerman, Dennis Bonatz, Maaike M. van der Sluijs, Johanna C. van der Bok, P. Tim Prins, Marcel Aebli, Alf Mews, Daniel Vanmaekelbergh, Maksym Kovalenko
Summary: Researchers have used in situ synchrotron-based small-angle X-ray scattering and optical absorption spectroscopy to gain new insights into the nucleation, growth, and self-assembly of lead halide perovskite nanocrystals. They found that dispersed 3 nm Cs[PbBr3] agglomerates are the key intermediate species, which slowly nucleate into crystals and release Cs[PbBr3] monomers for further growth. They also discovered the mechanism of spontaneous superlattice formation when the nanocrystals reach a critical size of 11.6 nm.
Article
Chemistry, Multidisciplinary
Yazi Liu, Yue Sun, En Zhao, Weiwei Yang, Jinkai Lin, Qiang Zhong, Haifeng Qi, Aixin Deng, Shaogui Yang, Huayang Zhang, Huan He, Shaomin Liu, Zupeng Chen, Shaobin Wang
Summary: This study reports the preparation of atomically dispersed Co-Ag dual-metal sites anchored on P-doped carbon nitride (Co1Ag1-PCN) via supramolecular and solvothermal approaches, which exhibit desirable performance for photocatalytic H-2 evolution from water splitting. The optimized Co1Ag1-PCN catalyst achieves a remarkable hydrogen production rate of 1190 mu mol g(-1) h(-1) with an apparent quantum yield (AQY) of 1.49% at 365 nm, surpassing most of the newly reported metal-N-coordinated photocatalysts. The enhanced photocatalytic activity is attributed to the synergistic effect of Co-Ag dual sites with exclusive coordination configuration of Co-N-6 and Ag-N2C2, which enhances the charge density and facilitates the formation of H* intermediates.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Wenjun Zhang, Shanshan Liu, Yue Yang, Haifeng Qi, Shibo Xi, Yanping Wei, Jie Ding, Zhu-Jun Wang, Qunxiang Li, Bin Liu, Zupeng Chen
Summary: Metal-organic framework catalysts offer new opportunities for CO2 electrocatalysis. Through density-functional theory calculations, Co-based porphyrin porous organic layers (Co-PPOLs) are predicted to have good activity for CO2 conversion due to their low *CO adsorption energy at Co-N-4 sites. Experimental results show that the prepared 2D Co-PPOLs with exclusive Co-N-4 sites exhibit high faradaic efficiency for CO production and CO selectivity, along with good stability and industrial-level current output in CO2 electrolysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Ruifan Tan, Ping Wang, Luyao Guo, Zupeng Chen, Ronghe Lin, Xiaoling Mou, Yunjie Ding
Summary: The shape of the carriers plays a significant role in the catalytic performance of metal-supported catalysts. This study investigates the impact of different shapes of ZrO2 (nanorods-like, spherical, and irregular nanoparticles) on the catalytic performance in methane dry reforming by dispersing Ni species. Various characterization techniques are used to analyze the fresh and spent catalysts. The reducibility of NiO species is found to follow the order of Ni/RZ.
Article
Engineering, Environmental
Jun Deng, Chi Zhou, Yue Yang, Bing Nan, Lin Dong, Lingchao Cai, Lina Li, Zhu-Jun Wang, Xiaofei Yang, Zupeng Chen
Summary: A mesoporous carbon nitride-supported ruthenium single-atom photocatalyst was developed for the selective cleavage of lignin C-C bonds. The catalyst exhibited high activity and selectivity under visible-light irradiation and room temperature. This work explores the potential of single-atom catalysts for the photocatalytic production of aromatics from renewable biomass feedstocks.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Cecilia Salah, Selene Cobo, Javier Perez-Ramirez, Gonzalo Guillen-Gosalbez
Summary: The increasing demand for single-use polymers requires the exploration of alternative waste treatment methods to achieve a circular economy. This study investigates the production of hydrogen from waste polymer gasification (wPG) as a means to reduce the environmental impact of plastic incineration and landfilling while generating valuable products. The carbon footprint and environmental sustainability of various H2 production routes, including wPG, natural gas, biomass, and water splitting, are assessed in relation to planetary boundaries. Results suggest that wPG combined with carbon capture and storage can effectively reduce the climate change impact compared to fossil-based and electrolytic routes. While the cost of wPG might be higher than fossil and biomass-based alternatives, it remains cheaper than electrolytic routes. Furthermore, a combination of pathways can meet the current global H2 demand without exceeding the studied planetary boundaries, indicating the potential role of H2 from plastics until chemical recycling technologies mature.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Qiao Tang, Jiang Wu, Xiang-Zhong Chen, Roger Sanchis-Gual, Andrea Veciana, Carlos Franco, Donghoon Kim, Ivan Surin, Javier Perez-Ramirez, Michele Mattera, Anastasia Terzopoulou, Ni Qin, Marija Vukomanovic, Bradley J. Nelson, Josep Luis, Salvador Pan
Summary: In this paper, oxygen vacancies (OVs) were introduced in Bi4Ti3O12 (BIT) nanosheets to enhance their piezo-photocatalytic performance. Compared to pristine BIT nanosheets, BIT with optimized OV concentration showed excellent piezo-photocatalytic activity, with a 2.2 times enhancement of the degradation rate constant for Rhodamine B (RhB). Density functional theory (DFT) calculations were used to investigate the effect of OVs on adsorption energy and Bader charges, providing insights into the underlying mechanism of OV enhanced piezo-photocatalytic activity. This study contributes to a deeper understanding of the regulation mechanism of OV enhanced piezo-photocatalytic activity and offers new approaches for designing high-performance piezo-photocatalysts.
Article
Chemistry, Physical
Huanyu Zhang, Giulia Paggiaro, Faruk Okur, Janis Huwiler, Claudia Cancellieri, Lars P. H. Jeurgens, Dmitry Chernyshov, Wouter van Beek, Maksym V. Kovalenko, Kostiantyn V. Kravchyk
Summary: The deployment of LLZO garnets as solid-state electrolytes for Li-metal solid-state batteries is hindered by the reactivity with water and carbon dioxide, leading to the formation of a contamination layer on the LLZO surface. High temperature annealing is studied as a thermal cleaning method, which effectively reduces the contamination but also results in the formation of a different phase on the LLZO surface. The impact of these factors on the performance of Li/LLZO/Li symmetrical cells was evaluated.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Julian Felix Baumgaertner, Michael Woerle, Christoph P. Guntlin, Frank Krumeich, Sebastian Siegrist, Valentina Vogt, Dragos C. Stoian, Dmitry Chernyshov, Wouter van Beek, Kostiantyn V. Kravchyk, Maksym V. Kovalenko
Summary: Pyrochlore-type iron (III) hydroxy fluorides (Pyr-IHF) are attractive as low-cost stationary energy storage materials due to their stable supply of constituent elements, high energy densities, and fast Li-ion diffusion. However, their commercial use is currently hindered by the high costs of synthesis and cathode architecture. In this study, a facile and cost-effective dissolution-precipitation synthesis method for Pyr-IHF from soluble iron (III) fluoride precursors is presented. The synthesized Pyr-IHF demonstrates high capacity retention of >80% after 600 cycles at a high current density of 1 A g(-1) without complex electrode engineering. Operando synchrotron X-ray diffraction is used to guide the selective synthesis of Pyr-IHF and investigate the effect of different water contents on rate capability. Li-ion diffusion is found to occur in the 3D hexagonal channels of Pyr-IHF formed by corner-sharing FeF6-x(OH)(x) octahedra.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Juan D. Medrano-Garcia, Vera Giulimondi, Amedeo Ceruti, Guido Zichittella, Javier Perez-Ramirez, Gonzalo Guillen-Gosalbez
Summary: This study evaluates the environmental potential and economics of recently developed catalytic ethane chlorination technologies for VCM synthesis. It finds that the current state of these technologies can lower production costs by 32% and could reduce the carbon footprint of VCM synthesis by up to 26% in the 2050 scenario.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Review
Chemistry, Multidisciplinary
Xinzhe Li, Sharon Mitchell, Yiyun Fang, Jun Li, Javier Perez-Ramirez, Jiong Lu
Summary: Heterogeneous single-cluster catalysts, which consist of metal clusters stabilized on supports, offer exciting prospects for enabling novel chemical reactions. However, synthetic and analytical challenges hinder a thorough understanding of their surface chemistry. This Review emphasizes the importance of considering the cluster environment and highlights the criticality of tailoring the entire catalytic ensemble to achieve stable and selective performance.
NATURE REVIEWS CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Abhinandan Nabera, Ioan-Robert Istrate, Antonio Jose Martin, Javier Perez-Ramirez, Gonzalo Guillen-Gosalbez
Summary: Ammonia and methanol production, heavily reliant on natural gas, have resulted in supply disruptions and significant CO2 emissions. Despite extensive research on low-carbon or green production routes, their adoption has been hindered by higher costs. However, the recent energy crisis in Europe has created an opportunity to transition towards greener production technologies.
Article
Chemistry, Multidisciplinary
Sebastiano C. D'Angelo, Antonio J. Martin, Selene Cobo, Diego Freire Ordonez, Gonzalo Guillen-Gosalbez, Javier Perez-Ramirez
Summary: Efforts to develop decentralized and sustainable schemes for ammonia production are yet to be evaluated. We found that small-scale systems based on electrocatalytic reduction of nitrogen powered by photovoltaic energy show promise in terms of environmental and economic criteria. NH3-leaf technology has the potential to outperform traditional production methods in terms of CO2-related Earth-system processes and human health.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Thomas Moragues, Sharon Mitchell, Dario Faust Akl, Javier Perez-Ramirez, Andrew deMello
Summary: Wet chemical approaches are widely used for preparing single-atom heterogeneous catalysts. However, the synthesis methods lack systematic considerations of different parameters' effects. In this study, a microfluidic platform is demonstrated for rapid and systematic syntheses of single-atom catalysts using various metal precursor-carrier combinations. The microfluidic approach allows precise control of concentrations and residence times, enabling the evaluation of metal precursor concentration's influence on the adsorption and dispersion of metal species. The method is confirmed to be applicable for different metals and carriers, opening possibilities for high-throughput screening and mechanistic studies in catalyst design.
