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B-doped Carbon Quantum Dots Anchored n/n-Junctioned Graphitic Carbon Nitride (g-C3N4) for CO2 Photoreduction 1

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2nd International Conference on Frontiers of Energy and Environmental engineering, CFEEE 2023

作者： Hiu, Jia Shen Phang, Sue Jiun Lee, Jiale Wong, Voon-Loong Tan, Lling-Lling School of Engineering and Physical Sciences Heriot-Watt University Malaysia Jalan Venna P5/2 Precinct 5 Putrajaya62200 Malaysia Multidisciplinary Platform of Advanced Engineering Chemical Engineering Discipline School of Engineering Monash University Jalan Lagoon Selatan Selangor Bandar Sunway47500 Malaysia

ISBN: (数字)9789819703722

ISBN: (纸本)9789819703715

The abundant use of fossil fuel resources, accompanied by climate change and global energy demands, has motivated the search for sustainable transformations of greenhouse gas CO2 into value-added chemical fuels. In present work, the production of methane (CH4) gas by photocatalytic CO2 reduction over a boron (B)-doped CQD (BCQD)-hybridized graphitic carbon nitride (g-C3N4) homojunction (CNH) nanocomposite was investigated. The CNH and undoped CQD-based g-C3N4 were also synthesized for the comparison of photoactivity towards CO2 conversion. All photoactivity assessments were performed under the irradiation of two 200 W LED lights at ambient temperature and pressure. The results revealed that BCQD/CNH obtained the highest photocatalytic efficiency by achieving a total CH4 yield of 28.12 μmol/(hr-gcatalyst) in 6 h, which was 49.61% and 30.99% higher than the pristine g-C3N4 and undoped CQD/CNH, respectively. A series of control experiments was also carried out in the absence of either photocatalysts, water or light for 6 h. BCQD/CNH was able to yield 54.56% of CH4 as compared to the control experiment without water. In contrast, the lowest CH4 yield of 1.122 μmol/hr was obtained in the absence of BCQD/CNH. The surface morphologies of CNH, CQD/CNH, and BCQD/CNH were also investigated via FESEM and TEM analysis. © The Author(s), under exclusive license to Springer Nature Singapore Pte Ltd. 2024.

关键词： Carbon dioxide

Complementary conjugated piezo-phototronic polarized blue TiO2 - KNN for piezophotocatalytic degradation of tetracycline enhanced under gentle oscillatory hydrodynamic disturbances

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Applied Catalysis B: Environmental 2023年第1期334卷

作者： Lee, Yong Jieh Chong, Wei-Kean Putri, Lutfi Kurnianditia Ng, Boon-Junn Tan, Lling-Lling Wu, Ta Yeong Chai, Siang-Piao Multidisciplinary Platform of Advanced Engineering Department of Chemical Engineering School of Engineering Monash University Malaysia Jalan Lagoon Selatan Selangor Bandar Sunway47500 Malaysia

Recently, tetracycline (TC) is classified as an emerging contaminant due to its rapid discharge into the environment from anthropogenic sources. Piezophotocatalysis offers a unique solution to degrade TCs by collaboratively harnessing both solar and hydro energy. However, practical applications have been hampered by the necessitation of high energy requirement ultrasonic baths. In this work, BT-KNN conjugates were investigated for piezophotocatalytic TC degradation. Under agitation conditions, characterization studies demonstrated an amplified photocurrent, diminished charge transfer resistance and reduced radiative recombination. Concomitantly, BT-KNN composites exhibit enhanced TC degradation and apparent rate constant with increased fluid disturbance frequencies, illustrating 91.3% degradation in 3 h under gentle 4 Hz oscillations. These hydrodynamic disturbances engender a propitious piezopolarization which modulated the junction band bending and ameliorated the interfacial charge transfer, intensifying its performance. Optimization studies further illustrates the tradeoff dynamics between high photoactivity of BT and high piezo-enhancement of KNN. © 2023 The Authors

关键词： Titanium dioxide

Identification and Design of Active Sites on Photocatalysts for the Direct Artificial Carbon Cycle

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Accounts of Materials Research 2022年第3期3卷 331-342页

作者： Jingxiang Low Jun Ma Jun Wan Wenbin Jiang Yujie Xiong Hefei National Laboratory for Physical Sciences at the Microscale School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefeiAnhui 230026China Multidisciplinary Platform of Advanced Engineering Chemical Engineering DisciplineSchool of EngineeringMonash UniversityBandar Sunway 47500 SelangorMalaysia

CONSPECTUS:Imitating the natural carbon cycle,the utilization of the carbon-based greenhouse gases(i.e.,carbon dioxide(CO_(2))and methane(CH_(4)))from the atmosphere as the carbon feedstocks for valuable fuel and chemical production represents a prospective strategy for achieving the sustainable development of human *** light of this,photocatalytic CO_(2)/CH_(4)conversions,which can directly harvest solar energy for the production of valuable fuels and chemicals,show gigantic potential for closing the loop of the artificial carbon *** the past several decades,immense progress has been made in this field,showing its practical ***,the photocatalytic conversion efficiency and selectivity of such reactions remain *** that the photocatalytic reaction is intimately related to the surface catalytic reaction on the active sites of the photocatalysts,the active site design has been proven to be effective for optimizing photocatalytic performance,yet the lack of effective techniques for the identification of the active sites,which is normally at the molecular level,greatly limits its potential in ***,with the rapid expansion in the field of materials science,a large number of advanced characterization techniques have been developed,equipping the materials scientist and chemist with powerful tools for unveiling the mask of the active sites on the ***,the active site design for the photocatalysts has undergone a ***,the identification and design of active sites have emerged as hot topics in catalysis and are expected to push forward development in the field of the artificial carbon cycle.

关键词： dioxide catalysis Active

Complementary Conjugated Piezo-Phototronic Polarized Blue Tio2 - Knn for Piezophotocatalytic Degradation of Tetracycline Enhanced Under Gentle Oscillatory Hydrodynamic Disturbances

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SSRN 2023年

作者： Lee, Yong Jieh Chong, Wei-Kean Putri, Lutfi Kurnianditia Ng, Boon-Junn Tan, Lling-Lling Wu, Ta Yeong Chai, Siang-Piao Multidisciplinary Platform of Advanced Engineering Chemical Engineering Discipline School of Engineering Monash University Malaysia Jalan Lagoon Selatan Bandar Sunway Selangor 47500 Malaysia

Recently, tetracycline (TC) is classified as an emerging contaminant due to its rapid discharge into the environment from anthropogenic sources. Piezophotocatalysis offers a unique solution to degrade TCs by collaboratively harnessing both solar and hydro energy. However, practical applications have been hampered by the necessitation of high energy requirement ultrasonic *** this work, BT-KNN conjugates were investigated for piezophotocatalytic TC degradation. Under agitation conditions, characterization studies demonstrated an amplified photocurrent, diminished charge transfer resistance and reduced radiative recombination. Concomitantly, BT-KNN composites exhibit enhanced TC degradation and apparent rate constant with increased fluid disturbance frequencies, illustrating 91.3 % degradation in 3 hours under gentle 4 Hz oscillations. These hydrodynamic disturbances engender a propitious piezopolarization which modulated the junction band bending and ameliorated the interfacial charge transfer, intensifying its performance. Optimization studies further illustrates the tradeoff dynamics between high photoactivity of BT and high piezo-enhancement of KNN. © 2023, The Authors. All rights reserved.

关键词： Titanium dioxide

Unveiling the Fundamental First Principles Insights of Single-Atom Transition Metal Photocatalysts for Carbon Dioxide Reduction

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SSRN 2024年

作者： Er, Chen-Chen Putri, Lutfi Kurnianditia Ang, Yee Sin Chai, Siang-Piao Multidisciplinary Platform of Advanced Engineering Department of Chemical Engineering School of Engineering Monash University Malaysia Jalan Lagoon Selatan Bandar Sunway Selangor Subang Jaya47500 Malaysia 8 Somapah Road 487372 Singapore

The search for new single-atom photocatalysts (SAPs) has garnered significant focus for CO2 reduction reaction (CO2RR) due to their maximum atom utilization efficiency. However, the rational design of SAPs remains elusive due to the lack of fundamental understanding behind the dynamic electron transfer between the anchored atoms and the semiconductor support. Herein, density functional theory calculations were performed to study the SAPs constituting transition metal (TM) in graphitic carbon nitride with a stoichiometry of C6N6 (gC6N6). A total of 26 single-atom elements from the TM group were investigated in this work. The in-depth analysis demonstrates that the selectivity for CO2RR over hydrogen evolution reaction (HER) is highly correlated with the degree of electrons transfer between the single TM atom and gC6N6. The coexistence of partially occupied states and empty states is essential for active CO2 adsorption for these SAPs. Overall, the findings from this work will steer experimental progress towards the design of efficient SAPs for CO2RR. © 2024, The Authors. All rights reserved.

关键词： Density functional theory

g-C_(3)N_(4) Photocatalysts:Utilizing Electron-Hole Pairs for Boosted Redox Capability in Water Splitting

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Energy Material Advances 2023年第1期4卷 304-330页

作者： Grayson Zhi Sheng Ling Valerie Bei-Yuan Oh Choon Yian Haw Lling-Lling Tan Wee-Jun Ong School of Energy and Chemical Engineering Xiamen University MalaysiaSepangSelangor Darul Ehsan43900Malaysia Center of Excellence for NaNo Energy&Catalysis Technology(CONNECT) Xiamen University MalaysiaSepangSelangor Darul Ehsan43900Malaysia State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Multidisciplinary Platform of Advanced Engineering Chemical Engineering DisciplineSchool of EngineeringMonash UniversityJalan Lagoon SelatanBandar SunwaySelangor47500Malaysia Shenzhen Research Institute of Xiamen University Shenzhen518057China Gulei Innovation Institute Xiamen UniversityZhangzhou363200China

Since the first discovery of solar-driven water splitting catalyzed by TiO_(2) semiconductors,extensive research works have been devoted over the ***,the design of a photocatalyst with dual redox potential is of prominent interest to fully utilize both photogenerated electrons and holes in the redox *** all,the coproduction of H_(2) and O_(2) from water using metal-free carbon nitride(g-C_(3)N_(4))has been viewed as a rising star in this ***,the hole-mediated oxidation reaction is commonly recognized as the rate-determining step,which drastically leads to poor overall water splitting *** top of that,rapid recombination and undesirable back reaction appeared as one of the challenging parts in overall water *** this review,the up-to-date advances in modified g-C_(3)N_(4)-based photocatalysts toward efficient overall water splitting are summarized,which are mainly classified into structural and defect engineering,single-atom catalysis,cocatalyst loading,and heterojunction *** review also addresses the underlying idea and concept to tackle the aforementioned problem with the use of emerging modification strategies,hence serving as the guiding star for future *** the outstanding breakthrough thus far,critical recommendations related to g-C_(3)N_(4) photocatalytic systems are prospected to pave the way toward the implementation in the practical energy production process.

关键词： process splitting catalyst

Novel materials and techniques for photocatalytic water splitting developed by Professor Kazunari Domen

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Chinese Journal of Catalysis 2025年第1期68卷 1-50页

作者： Yaqiang Wu Jianuo Li Wei-Kean Chong Zhenhua Pan Qian Wang Graduate School of Engineering Nagoya UniversityFuro-choChikusa-kuNagoya 464-8603Japan State Key Laboratory of Crystal Materials Institute of Crystal MaterialsShandong UniversityJinan 250100ShandongChina Multidisciplinary Platform of Advanced Engineering Department of Chemical EngineeringSchool of EngineeringMonash University MalaysiaJalan Lagoon Selatan47500 Bandar SunwaySelangorMalaysia Department of Applied Chemistry Graduate School of EngineeringUniversity of HyogoHimejiHyogo 671-2280Japan Institute for Advanced Research Nagoya UniversityFuro-choChikusa-kuNagoya 464-8601Japan

Professor Kazunari Domen at the Shinshu University and the University of Tokyo has pioneered materials and techniques for solar-driven water splitting using photocatalysts,a promising technology for contributing to the construction of a sustainable and carbon-neutral *** this paper,we summarize his groundbreaking contributions to photocatalytic water splitting and,more broadly,photocatalytic *** highlight various novel functional photocatalytic materials,including oxides,(oxy)nitrides,and oxysulfides,along with innovative techniques such as cocatalyst engineering and Z-scheme system construction developed by the Domen *** team has also pioneered readily accessible and cost-effective photo(electro)chemical device fabrication methods,such as the particle-transfer method and thin-film-transfer ***,their research has made significant contributions to understanding the(photo)catalytic mechanisms using advanced characterization *** with his research team,Professor Domen has set many milestones in the field of photocatalytic overall water splitting,notably demonstrating the first scalable and stable 100 m^(2)solar H_(2)production system using only water and *** work has revealed the potential for practical solar H2 production from water and sunlight,and highlighted the application of fundamental principles,combined with chemical and materials science tools,to design effective photocatalytic *** this review,we focus on his research and the foundational design principles that can inspire the development of efficient photocatalytic systems for water splitting and solar fuel *** building on his contributions,we anticipate a significant impact on addressing major global energy challenges.

关键词： Photocatalysis Water splitting Solar H_(2)production Solar energy conversion Artificial photosynthesis

Diesel Pollution Blues? Blue Tio2 with Tunable Oxygen-Vacancy Defects for Enhanced Photocatalytic Diesel Oil Degradation

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SSRN 2022年

作者： Lee, Yong Jieh Putri, Lutfi Kurnianditia Ng, Boon-Junn Tan, Lling-Lling Wu, Ta Yeong Chai, Siang-Piao Multidisciplinary Platform of Advanced Engineering Chemical Engineering Discipline School of Engineering Monash University Jalan Lagoon Selatan Bandar Sunway Selangor 47500 Malaysia

The proliferation of marine petroleum exploitation has culminated in the undesired release of oils into the aquatic ecosystem, causing detrimental environmental effects. Photocatalysis proffers a solution to degrade recalcitrant diesel oil utilizing abundant solar energy, in which TiO2 is the perennial photocatalyst of choice. However, it suffers from the low utilization of the light spectrum and the rapid recombination of photogenerated charge carriers. In this work, oxygen-vacancy-rich blue TiO2 was employed to overcome the shortcomings of TiO2 in diesel oil degradation which has historically not been attempted. These oxygen vacancies induce favourable mid gap states to extend the optical absorption capabilities and enrich the photocatalyst charge density. Additionally, oxygen vacancies enhance the separation of electron hole pairs by acting as trap states, evident from increased trap-mediated capture fluorescence. Consequently, a 1.60-fold enhancement of diesel oil degradation performance compared to pristine TiO2 was observed. Mechanistic insights revealed the restructuring of diesel alkane distribution upon degradation corollary to the cleavage of hydrocarbon chains, illustrating that short alkanes experience a greater susceptibility to degradation compared to long alkanes. GC-MS analysis elucidates that shorter chained alkanes, alkenes, alcohols and cycloalkanes are produced as a product of the degradation. © 2022, The Authors. All rights reserved.

关键词： Titanium dioxide

Cyano Group Modified Graphitic Carbon Nitride with K Intercalation for Sustainable Photodegradation of Pharmaceutical Waste

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SSRN 2022年

作者： Lee, Jiale Tan, Xin-Yu Ng, Boon-Junn Chai, Siang-Piao Tan, Lling-Lling Multidisciplinary Platform of Advanced Engineering Chemical Engineering Discipline School of Engineering Monash University Jalan Lagoon Selatan Bandar Sunway Selangor47500 Malaysia

In the past few decades, pharmaceutical and personal care products (PPCPs) pollutants in aquatic environment have risen as an alarming concern. The elimination of these compounds via the conventional treatment processes is challenging owing to the low molecular weight and strong hydrophilicity of PPCPs. The non-toxic graphitic carbon nitride (g-C 3 N 4 ) is a highly promising material for sustainable environmental remediation but suffers from key bottlenecks of rapid charge recombination and poor light absorption capacity. Herein, the photocatalytic performance of g-C 3 N 4 is significantly improved by a facile alkali treatment with potassium hydroxide (KOH). A study on the degradation of acetaminophen (ACE) over potassium-intercalated g-C 3 N 4 (K-CN) with varying KOH concentration was carried out. With an optimum amount of KOH used, 1.2K-CN exhibited a 2.51-fold increase in degradation efficiency and 5.29-fold enhancement in the corresponding pseudo-first-order rate constant as compared to pristine g-C 3 N 4 . The superior photocatalytic activity of 1.2K-CN is ascribed to the formation of cyano group (C≡N) and intercalation of K atoms in g-C 3 N 4 , which were corroborated through various characterization techniques to reveal the greater light absorbance, narrowed band gap, effective transmission of photogenerated charge carriers and suppressed electron-hole recombination. In addition, superoxide anions (•O 2 − ) were shown to be the leading reactive oxidative species contributing to the degradation reaction, followed by photoinduced holes (h + ) and hydroxyl (•OH) radicals. Lastly, a plausible pathway of the ACE photodegradation mechanism over 1.2K-CN is proposed. Overall, this work provides a simple yet effective approach to boost the performance of g-C 3 N 4 and it is anticipated to initiate further research in sustainable pharmaceutical wastewater degradation. © 2022, The Authors. All rights reserved.

关键词： Carbon nitride