物理化学学报最新文献

{"title":"Construction of ZnCoP/CdLa2S4 Schottky Heterojunctions for Enhancing Photocatalytic Hydrogen Evolution","authors":"Jianyin He ,&nbsp;Liuyun Chen ,&nbsp;Xinling Xie ,&nbsp;Zuzeng Qin ,&nbsp;Hongbing Ji ,&nbsp;Tongming Su","doi":"10.3866/PKU.WHXB202404030","DOIUrl":"10.3866/PKU.WHXB202404030","url":null,"abstract":"<div><div>Photocatalytic hydrogen evolution by heterojunction photocatalysts is considered an effective way to address environmental and energy crises. In this work, a novel ZnCoP/CdLa₂S₄ Schottky heterojunction was prepared <em>via</em> a physical mixing method assisted by water bath heating and used to enhance the efficiency of photocatalytic hydrogen production. Owing to the higher work function and metallic conductivity of ZnCoP, the photoinduced electrons can transfer from CdLa₂S₄ to ZnCoP through the ZnCoP/CdLa₂S₄ interface, which suppresses the recombination of photoinduced electrons and holes. Moreover, the Schottky heterojunction formed at the interface between ZnCoP and CdLa₂S₄ inhibits electron backflow from ZnCoP to CdLa₂S₄, which further promotes the separation of electron-hole pairs. Meanwhile, the ZnCoP/CdLa₂S₄ heterojunction exhibited enhanced visible light absorption compared to CdLa₂S₄. In addition, ZnCoP acts as an electron acceptor and hydrogen evolution active site. The synergistic effect of the tight ZnCoP/CdLa₂S₄ interface, the higher work function and metallic conductivity of ZnCoP, and the formation of Schottky junctions significantly enhance the photocatalytic hydrogen production evolution performance of CdLa₂S₄. When the amount of ZnCoP was 30 wt% (wt%, mass fraction), the 30ZCP/CLS composite showed the highest photocatalytic performance, and the hydrogen production rate reached 10.26 mmol·g⁻¹·h⁻¹ under visible light irradiation and with Na₂S and Na₂SO₃ as sacrificial agents, which was 7.7 times that of CdLa₂S₄. Combined with the activity data and characterization results, a potential mechanism for photocatalytic hydrogen production over ZnCoP/CdLa₂S₄ Schottky heterojunctions was proposed.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (98KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2404030"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145963","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient Photocatalytic Production of H2O2 over ZnO/D-A Conjugated Polymer S-Scheme Heterojunction and Charge Transfer Dynamics Investigation","authors":"You Wu ,&nbsp;Chang Cheng ,&nbsp;Kezhen Qi ,&nbsp;Bei Cheng ,&nbsp;Jianjun Zhang ,&nbsp;Jiaguo Yu ,&nbsp;Liuyang Zhang","doi":"10.3866/PKU.WHXB202406027","DOIUrl":"10.3866/PKU.WHXB202406027","url":null,"abstract":"<div><div>Photocatalytic technology harnesses clean, non-polluting solar energy to synthesize hydrogen peroxide (H₂O₂). In this study, ZnO/PBD S-scheme heterojunction composites, featuring ZnO nanoparticles on a donor-acceptor conjugated polymer substrate (PBD), were synthesized <em>via</em> the Suzuki-Miyaura reaction and hydrothermal method. The optimal ZnO/PBD composite achieved an H₂O₂ production efficiency of 4.07 mmol·g⁻¹·h⁻¹, which is 5.4 times higher than that of pristine ZnO. This significant enhancement is attributed to the formation of S-scheme heterojunctions. The successful construction of S-scheme heterojunctions was confirmed through UV-visible absorption spectroscopy and <em>in situ</em> irradiated X-ray photoelectron spectroscopy. Steady-state photoluminescence and femtosecond transient absorption (fs-TA) spectroscopies identified and verified the presence of defect states in ZnO. These defect states trap photogenerated electrons, adversely affecting the photocatalytic reaction. However, the S-scheme heterojunction effectively promotes the separation and transfer of electrons, mitigating this issue. The measured lifetimes of photogenerated electrons in these defect states, as determined by fitted fs-TA decay kinetics, provided further evidence of the carrier transfer mechanism in S-scheme heterojunctions. This work introduces a novel approach for studying organic/inorganic S-scheme heterojunctions using fs-TA spectroscopy.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (72KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2406027"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145015","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Improved Photo-Carrier Transfer by an Internal Electric Field in BiOBr/Nrich C3N5 3D/2D S-Scheme Heterojunction for Efficiently Photocatalytic Micropollutant Removal","authors":"Changjun You ,&nbsp;Chunchun Wang ,&nbsp;Mingjie Cai ,&nbsp;Yanping Liu ,&nbsp;Baikang Zhu ,&nbsp;Shijie Li","doi":"10.3866/PKU.WHXB202407014","DOIUrl":"10.3866/PKU.WHXB202407014","url":null,"abstract":"<div><div>Photocatalytic wastewater decontamination techniques hold eminent promise in mitigating environmental deterioration, yet the lack of distinctive photocatalysts prevents their further large-scale application. Herein, an S-scheme heterojunction photocatalyst BiOBr/C₃N₅ (BBN) was fabricated for efficiently dislodging micropollutants under visible light. Among the BBN samples, the optimal BBN-2 demonstrated exceptional activity in photocatalytic TC removal with a rate constant of 0.0139 min^‒1, which surpassed that of pure BiOBr and C₃N₅ by 0.6 and 2.8 times, respectively. The spatially segregated photoredox sites and efficient photo-carrier separation propelled by an internal electric field are found to play a cardinal role in promoting photoreaction kinetics. Moreover, BBN-2 exhibited remarkable resistance to environmental interference and stability, retaining a high activity level after five runs. Through active radical detection, •O₂^‒, h⁺ and •OH were identified as the primary active species in the photocatalytic reaction process. This research would encourage the exploration of C₃N₅-based photocatalysts for environmental protection.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (91KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2407014"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145019","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Accelerated Interfacial Electron Transfer in Perovskite Solar Cell by Ammonium Hexachlorostannate Modification and fs-TAS Investigation","authors":"Jizhou Liu ,&nbsp;Chenbin Ai ,&nbsp;Chenrui Hu ,&nbsp;Bei Cheng ,&nbsp;Jianjun Zhang","doi":"10.3866/PKU.WHXB202402006","DOIUrl":"10.3866/PKU.WHXB202402006","url":null,"abstract":"<div><div>Organic-inorganic halide perovskite solar cells (PSCs) have received widespread attention due to their outstanding photovoltaic performance and straightforward preparation process. However, charge recombination at the interface is a crucial factor limiting further enhancement of the power conversion efficiency (PCE) of the PSCs. In this study, we report the interfacial modification between the electron transport layer and the perovskite film (PSK) using ammonium hexachlorostannate (AH) crystals synthesized <em>via</em> the room temperature spin-coating method. AH as an inorganic tin-based perovskite material, can passivate defects in the PSK and establish a better lattice match, thereby enhancing the quality and crystallinity of the PSK. Kelvin probe force microscopy results confirm that AH promotes the directional migration of photogenerated electrons. Femtosecond transient absorption spectroscopy results verify that AH effectively shortens the lifetime of electron extraction and facilitates interfacial electron transfer. Based on the benefits of AH modification, AH-based PSCs exhibit higher PCE and reduced hysteresis effect.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (104KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2402006"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143144996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Improving Photocatalytic H2O2 Production over iCOF/Bi2O3 S-Scheme Heterojunction in Pure Water via Dual Channel Pathways","authors":"Yang Xia ,&nbsp;Kangyan Zhang ,&nbsp;Heng Yang ,&nbsp;Lijuan Shi ,&nbsp;Qun Yi","doi":"10.3866/PKU.WHXB202407012","DOIUrl":"10.3866/PKU.WHXB202407012","url":null,"abstract":"<div><div>Solar photocatalysis is a green, economical, and sustainable method for H₂O₂ synthesis, which has been regarded as the most promising alternative to the traditional anthraquinone oxidation method. However, single-component photocatalyst exhibits moderate activity owing to the limited light-harvesting range, fast charge recombination and inadequate redox capacity. Moreover, the addition of sacrificial agents is required in the reaction system. Herein, we present the development of an S-scheme heterojunction, achieved through photodepositing Bi₂O₃ nanoparticles (BO) on ionic covalent organic framework nanofiber (iCOF). The optimized photocatalyst iCOF/BO10 shows the highest H₂O₂ production performance in pure water, achieving an H₂O₂ yield of 9.76 mmolꞏg⁻¹ꞏh⁻¹ with an apparent quantum yield (AQY) of 5.5% at 420 nm. This photocatalytic performance is approximately 2.2 and 5.6 times as high as that of pristine iCOF and BO, respectively. In-depth characterizations including <em>in situ</em> irradiated XPS, DFT-calculations, active species trapping experiments and <em>in situ</em> DRIFTS, reveal that the obtained sample not only facilitates charge carrier separation and enhances light absorption capability, but also maximizes the redox ability to concurrently achieve indirect 2e⁻ ORR and 4e⁻ WOR for H₂O₂ production. Additionally, the generated O₂ from the 4e⁻ WOR is capable of accelerating the reaction kinetics for H₂O₂ formation <em>via</em> the indirect 2e⁻ ORR pathway, enabling overall photocatalytic H₂O₂ synthesis. This work provides a new insight into creating innovative catalysts for achieving high-efficiency photosynthesis of H₂O₂.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (84KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2407012"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Highly Efficient InOOH/ZnIn2S4 Hollow Sphere S-Scheme Heterojunction with 0D/2D Interface for Enhancing Photocatalytic CO2 Conversion","authors":"Jiaxing Cai ,&nbsp;Wendi Xu ,&nbsp;Haoqiang Chi ,&nbsp;Qian Liu ,&nbsp;Wa Gao ,&nbsp;Li Shi ,&nbsp;Jingxiang Low ,&nbsp;Zhigang Zou ,&nbsp;Yong Zhou","doi":"10.3866/PKU.WHXB202407002","DOIUrl":"10.3866/PKU.WHXB202407002","url":null,"abstract":"<div><div>S-scheme heterojunction system represents a highly efficient strategy for photocatalytic applications as it can simultaneously facilitate photogenerated charge carrier separation and enhance the reduction-oxidation potentials of the photocatalyst. Despite its gigantic potential, the photocatalytic CO₂ conversion efficiency of the S-scheme heterojunction remains limited mainly attributed to the sluggish interfacial charge carrier migration and poor light utilization efficiency. Herein, we prepare an InOOH/ZnIn₂S₄ hollow sphere S-scheme heterojunction with 0D/2D contact interface for enhancing photocatalytic CO₂ conversion performance. Specifically, the hollow sphere morphology can cause the multireflection of incident light within the photocatalyst leading to enhanced light absorption of the photocatalyst. In addition, the 0D/2D contact interface can facilitate the photogenerated charge carrier migration transfer over the InOOH/ZnIn₂S₄ S-scheme heterojunction. Furthermore, combining <em>in situ</em> irradiated X-ray photoelectron spectroscopy (ISIXPS) characterization and radicals trapping test, it is affirmed the accumulation of photogenerated holes and electrons respectively on InOOH and ZnIn₂S₄, which is beneficial for the effective utilization of photogenerated charge carriers. As a result, the photocatalytic CO₂ conversion performance of the optimized InOOH/ZnIn₂S₄ is <em>ca.</em> 25.8 times higher than that of pristine ZnIn₂S₄. Our reported results demonstrate a facile yet effective strategy for enhancing the interfacial photogenerated charge carrier migration and light utilization efficiency of S-scheme heterojunction.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (98KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2407002"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Construction of Electron Bridge and Activation of MoS2 Inert Basal Planes by Ni Doping for Enhancing Photocatalytic Hydrogen Evolution","authors":"Qin Hu ,&nbsp;Liuyun Chen ,&nbsp;Xinling Xie ,&nbsp;Zuzeng Qin ,&nbsp;Hongbing Ji ,&nbsp;Tongming Su","doi":"10.3866/PKU.WHXB202406024","DOIUrl":"10.3866/PKU.WHXB202406024","url":null,"abstract":"<div><div>Photocatalytic hydrogen production is one of the effective ways to address environmental pollution and energy crises. Herein, Ni_<em>x</em>-MoS₂/ZnIn₂S₄ heterojunctions were constructed to improve the separation efficiency of photogenerated electrons and holes and increase the number of active sites for hydrogen evolution. According to the catalyst characterization and theoretical calculations, the Ni at the interface between Ni_<em>x</em>-MoS₂ and ZnIn₂S₄ can act as a bridge for charge transfer, the Ni―S bond is the active site for H₂O dissociation, and the S site near the S vacancy on the Ni_<em>x</em>-MoS₂ surface enhances the hydrogen evolution reaction. Benefiting from the synergistic effect of the S vacancy and the Ni-doped MoS₂ cocatalyst, the optimal Ni_0.08-MoS₂/ZnIn₂S₄ exhibited the best hydrogen production rate of 7.13 mmol∙h⁻¹∙g⁻¹, which is 12.08 times than that of ZnIn₂S₄. This work provides a new strategy for enhancing photocatalytic efficiency through the synergistic effect of surface vacancies and doping and the optimization of heterojunctions.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (135KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2406024"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145958","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Simultaneously Improving Inter-Plane Crystallization and Incorporating K Atoms in g-C3N4 Photocatalyst for Highly-Efficient H2O2 Photosynthesis","authors":"Wei Zhong ,&nbsp;Dan Zheng ,&nbsp;Yuanxin Ou,&nbsp;Aiyun Meng,&nbsp;Yaorong Su","doi":"10.3866/PKU.WHXB202406005","DOIUrl":"10.3866/PKU.WHXB202406005","url":null,"abstract":"<div><div>Graphitic carbon nitride (g-C₃N₄) has gained growing attention in hydrogen peroxide (H₂O₂) photosynthesis, but the low activity of two-electron oxygen reduction reaction (2e⁻-ORR) still restricts its photocatalytic H₂O₂-generation performance. Herein, traditional g-C₃N₄ photocatalysts are recrystallized on KI crystal surfaces by a secondary calcination route to synthesize K incorporated highly-crystalline g-C₃N₄ photocatalysts. The synthesized CN-K photocatalyst exhibits improved inter-plane crystallization, narrowed bandgap structure, and smaller particle size from 20 to 50 nm. Moreover, the incorporated K atoms, as excellent catalytic sites, can enhance O₂ adsorption and stabilize the *OOH intermediates, thus improving the 2e⁻-ORR activity of the K incorporated high-crystallization g-C₃N₄ photocatalysts. Consequently, the optimized CN-K(1:6) photocatalyst exhibits a remarkably improved H₂O₂-generation rate of 7.8 mmol·L⁻¹·h⁻¹ with an AQE value of 5.17% at 420 nm, outperforming the traditional g-C₃N₄ sample by a factor of 220. This work uncovers the roles of heteroatoms in promoting the 2e⁻-ORR selectivity of the g-C₃N₄ photocatalyst, and offers novel insights to construct highly-active g-C₃N₄-based materials for H₂O₂ photosynthesis.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (65KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2406005"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hierarchical S-Scheme Heterojunction of Red Phosphorus Nanoparticles Embedded Flower-like CeO2 Triggering Efficient Photocatalytic Hydrogen Production","authors":"Chenye An ,&nbsp;Abiduweili Sikandaier ,&nbsp;Xue Guo ,&nbsp;Yukun Zhu ,&nbsp;Hua Tang ,&nbsp;Dongjiang Yang","doi":"10.3866/PKU.WHXB202405019","DOIUrl":"10.3866/PKU.WHXB202405019","url":null,"abstract":"<div><div>Designing heterojunctions using two semiconductors with aligned band structures is a promising strategy for solar energy-driven photocatalytic hydrogen production. Particularly, S-scheme heterojunctions exhibit significant promise for accelerating spatial separation and migration of photoexcited charge carriers while maintaining strong redox capacity. Herein, a hierarchical S-scheme composite of red phosphorus (RP) nanoparticles decorated flower-like CeO₂ (CeO₂/RP) was synthesized <em>via</em> the chemical vapor deposition process. Under simulated solar light irradiation, the optimized CeO₂/RP S-scheme heterojunction exhibited a highly efficient photocatalytic hydrogen production rate of 297.8 μmolꞏh⁻¹ꞏg⁻¹, which is approximately 8.8 and 5.7 times greater than that of pure CeO₂ and RP, respectively. After decoration with RP, the optical absorption of CeO₂/RP is greatly expanded to the visible light region. The effective photocatalytic performance can be primarily attributed to the presence of interfacial P―O―Ce bonds providing charge transfer pathways, as well as the development of a built-in electric field between CeO₂ and RP at the intimate interface. The photogenerated electrons follow an S-scheme mechanism, the electric field drives directional charge transfer from the conduction band (CB) of CeO₂ to the valence band (VB) of RP upon exposure to light, thus enabling the retention of photoexcited electrons and holes with higher redox potential at the CB of RP and the VB of CeO₂, respectively. This work provides a novel vision in the fabrication of S-scheme photocatalytic heterojunction systems with great photocatalytic hydrogen production performance.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (102KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2405019"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145014","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Construction of 4-Amino-1H-imidazole-5-carbonitrile Modified Carbon Nitride-based Donor-Acceptor Photocatalyst for Efficient Photocatalytic Hydrogen Evolution","authors":"Jingzhao Cheng ,&nbsp;Shiyu Gao ,&nbsp;Bei Cheng ,&nbsp;Kai Yang ,&nbsp;Wang Wang ,&nbsp;Shaowen Cao","doi":"10.3866/PKU.WHXB202406026","DOIUrl":"10.3866/PKU.WHXB202406026","url":null,"abstract":"<div><div>Photocatalytic hydrogen generation through water splitting driven by solar energy is regarded as a highly promising strategy to tackle the challenges of the energy crisis and environmental contamination. Tuning the electronic properties and band structures of photocatalysts is critical to improving the efficiency of charge separation and the activity of hydrogen production. Herein, donor-acceptor modified polymeric carbon nitride (CN)-based copolymers are synthesized <em>via</em> the introduction of 4-amino-1H-imidazole-5-carbonitrile (AICN) into the molecular skeleton of CN. The incorporation of electron donor AICN units can broaden the <em>π</em>-conjugated system and promote the spatial charge separation in the catalysts, thus resulting in enhanced light utilization and improved intramolecular charge carrier transfer rate. As a consequence, the AICN modified CN samples exhibit an increased photocatalytic hydrogen evolution rate, and the optimal photocatalytic activity can reach 3204 μmol·h⁻¹·g⁻¹. This molecular engineering strategy provides an effective avenue to develop high-performance CN-based photocatalysts for hydrogen evolution.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (63KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2406026"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145018","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}