物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202402006
Jizhou Liu , Chenbin Ai , Chenrui Hu , Bei Cheng , Jianjun Zhang
{"title":"Accelerated Interfacial Electron Transfer in Perovskite Solar Cell by Ammonium Hexachlorostannate Modification and fs-TAS Investigation","authors":"Jizhou Liu , Chenbin Ai , Chenrui Hu , Bei Cheng , 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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202407012
Yang Xia , Kangyan Zhang , Heng Yang , Lijuan Shi , Qun Yi
{"title":"Improving Photocatalytic H2O2 Production over iCOF/Bi2O3 S-Scheme Heterojunction in Pure Water via Dual Channel Pathways","authors":"Yang Xia , Kangyan Zhang , Heng Yang , Lijuan Shi , 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 H<sub>2</sub>O<sub>2</sub> 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 Bi<sub>2</sub>O<sub>3</sub> nanoparticles (BO) on ionic covalent organic framework nanofiber (iCOF). The optimized photocatalyst iCOF/BO10 shows the highest H<sub>2</sub>O<sub>2</sub> production performance in pure water, achieving an H<sub>2</sub>O<sub>2</sub> yield of 9.76 mmolꞏg<sup>−1</sup>ꞏh<sup>−1</sup> 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<sup>−</sup> ORR and 4e<sup>−</sup> WOR for H<sub>2</sub>O<sub>2</sub> production. Additionally, the generated O<sub>2</sub> from the 4e<sup>−</sup> WOR is capable of accelerating the reaction kinetics for H<sub>2</sub>O<sub>2</sub> formation <em>via</em> the indirect 2e<sup>−</sup> ORR pathway, enabling overall photocatalytic H<sub>2</sub>O<sub>2</sub> synthesis. This work provides a new insight into creating innovative catalysts for achieving high-efficiency photosynthesis of H<sub>2</sub>O<sub>2</sub>.</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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202407002
Jiaxing Cai , Wendi Xu , Haoqiang Chi , Qian Liu , Wa Gao , Li Shi , Jingxiang Low , Zhigang Zou , Yong Zhou
{"title":"Highly Efficient InOOH/ZnIn2S4 Hollow Sphere S-Scheme Heterojunction with 0D/2D Interface for Enhancing Photocatalytic CO2 Conversion","authors":"Jiaxing Cai , Wendi Xu , Haoqiang Chi , Qian Liu , Wa Gao , Li Shi , Jingxiang Low , Zhigang Zou , 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 CO<sub>2</sub> 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/ZnIn<sub>2</sub>S<sub>4</sub> hollow sphere S-scheme heterojunction with 0D/2D contact interface for enhancing photocatalytic CO<sub>2</sub> 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/ZnIn<sub>2</sub>S<sub>4</sub> 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 ZnIn<sub>2</sub>S<sub>4</sub>, which is beneficial for the effective utilization of photogenerated charge carriers. As a result, the photocatalytic CO<sub>2</sub> conversion performance of the optimized InOOH/ZnIn<sub>2</sub>S<sub>4</sub> is <em>ca.</em> 25.8 times higher than that of pristine ZnIn<sub>2</sub>S<sub>4</sub>. 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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202406024
Qin Hu , Liuyun Chen , Xinling Xie , Zuzeng Qin , Hongbing Ji , Tongming Su
{"title":"Construction of Electron Bridge and Activation of MoS2 Inert Basal Planes by Ni Doping for Enhancing Photocatalytic Hydrogen Evolution","authors":"Qin Hu , Liuyun Chen , Xinling Xie , Zuzeng Qin , Hongbing Ji , 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<sub><em>x</em></sub>-MoS<sub>2</sub>/ZnIn<sub>2</sub>S<sub>4</sub> 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<sub><em>x</em></sub>-MoS<sub>2</sub> and ZnIn<sub>2</sub>S<sub>4</sub> can act as a bridge for charge transfer, the Ni―S bond is the active site for H<sub>2</sub>O dissociation, and the S site near the S vacancy on the Ni<sub><em>x</em></sub>-MoS<sub>2</sub> surface enhances the hydrogen evolution reaction. Benefiting from the synergistic effect of the S vacancy and the Ni-doped MoS<sub>2</sub> cocatalyst, the optimal Ni<sub>0.08</sub>-MoS<sub>2</sub>/ZnIn<sub>2</sub>S<sub>4</sub> exhibited the best hydrogen production rate of 7.13 mmol∙h<sup>−1</sup>∙g<sup>−1</sup>, which is 12.08 times than that of ZnIn<sub>2</sub>S<sub>4</sub>. 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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202406005
Wei Zhong , Dan Zheng , Yuanxin Ou, Aiyun Meng, Yaorong Su
{"title":"Simultaneously Improving Inter-Plane Crystallization and Incorporating K Atoms in g-C3N4 Photocatalyst for Highly-Efficient H2O2 Photosynthesis","authors":"Wei Zhong , Dan Zheng , Yuanxin Ou, Aiyun Meng, Yaorong Su","doi":"10.3866/PKU.WHXB202406005","DOIUrl":"10.3866/PKU.WHXB202406005","url":null,"abstract":"<div><div>Graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) has gained growing attention in hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) photosynthesis, but the low activity of two-electron oxygen reduction reaction (2e<sup>−</sup>-ORR) still restricts its photocatalytic H<sub>2</sub>O<sub>2</sub>-generation performance. Herein, traditional g-C<sub>3</sub>N<sub>4</sub> photocatalysts are recrystallized on KI crystal surfaces by a secondary calcination route to synthesize K incorporated highly-crystalline g-C<sub>3</sub>N<sub>4</sub> 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 O<sub>2</sub> adsorption and stabilize the *OOH intermediates, thus improving the 2e<sup>−</sup>-ORR activity of the K incorporated high-crystallization g-C<sub>3</sub>N<sub>4</sub> photocatalysts. Consequently, the optimized CN-K(1:6) photocatalyst exhibits a remarkably improved H<sub>2</sub>O<sub>2</sub>-generation rate of 7.8 mmol·L<sup>−1</sup>·h<sup>−1</sup> with an AQE value of 5.17% at 420 nm, outperforming the traditional g-C<sub>3</sub>N<sub>4</sub> sample by a factor of 220. This work uncovers the roles of heteroatoms in promoting the 2e<sup>−</sup>-ORR selectivity of the g-C<sub>3</sub>N<sub>4</sub> photocatalyst, and offers novel insights to construct highly-active g-C<sub>3</sub>N<sub>4</sub>-based materials for H<sub>2</sub>O<sub>2</sub> 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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202405019
Chenye An , Abiduweili Sikandaier , Xue Guo , Yukun Zhu , Hua Tang , Dongjiang Yang
{"title":"Hierarchical S-Scheme Heterojunction of Red Phosphorus Nanoparticles Embedded Flower-like CeO2 Triggering Efficient Photocatalytic Hydrogen Production","authors":"Chenye An , Abiduweili Sikandaier , Xue Guo , Yukun Zhu , Hua Tang , 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 CeO<sub>2</sub> (CeO<sub>2</sub>/RP) was synthesized <em>via</em> the chemical vapor deposition process. Under simulated solar light irradiation, the optimized CeO<sub>2</sub>/RP S-scheme heterojunction exhibited a highly efficient photocatalytic hydrogen production rate of 297.8 μmolꞏh<sup>−1</sup>ꞏg<sup>−1</sup>, which is approximately 8.8 and 5.7 times greater than that of pure CeO<sub>2</sub> and RP, respectively. After decoration with RP, the optical absorption of CeO<sub>2</sub>/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 CeO<sub>2</sub> 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 CeO<sub>2</sub> 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 CeO<sub>2</sub>, 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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202406026
Jingzhao Cheng , Shiyu Gao , Bei Cheng , Kai Yang , Wang Wang , Shaowen Cao
{"title":"Construction of 4-Amino-1H-imidazole-5-carbonitrile Modified Carbon Nitride-based Donor-Acceptor Photocatalyst for Efficient Photocatalytic Hydrogen Evolution","authors":"Jingzhao Cheng , Shiyu Gao , Bei Cheng , Kai Yang , Wang Wang , 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<sup>−1</sup>·g<sup>−1</sup>. 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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202407013
Fei Xie , Chengcheng Yuan , Haiyan Tan , Alireza Z. Moshfegh , Bicheng Zhu , Jiaguo Yu
{"title":"d-Band Center Regulated O2 Adsorption on Transition Metal Single Atoms Loaded COF: A DFT Study","authors":"Fei Xie , Chengcheng Yuan , Haiyan Tan , Alireza Z. Moshfegh , Bicheng Zhu , Jiaguo Yu","doi":"10.3866/PKU.WHXB202407013","DOIUrl":"10.3866/PKU.WHXB202407013","url":null,"abstract":"<div><div>Covalent organic framework (COF) materials are promising photocatalysts because of their fantastic structural and physicochemical features. To enhance photocatalytic performance, numerous metal single atoms (MSA) are loaded on COF to improve molecule adsorption. However, the inherent mechanisms and dominant factors of the heightened adsorption property are not deeply unveiled. Herein, four MSA-COF systems were constructed by severally introducing Fe, Co, Ni, and Cu single atoms in monolayer TpBpy-COF. The effect of various metal atoms modification on the electronic property and O<sub>2</sub> adsorption of COF was investigated using density functional theory calculations. The results show that the metal atoms are bonded to the pyridinic N atoms, forming stable MSA-COF configurations. The anchoring of metal atoms reduces the band gap and raises the Fermi level of COF. Moreover, as the atomic number of the metals increases, the <em>d</em> orbitals of the metal atoms gradually move to lower energy levels, manifesting a negative shift of the <em>d</em>-band centers. After metal atoms loading, the weak physical adsorption of O<sub>2</sub> on pristine COF is converted to robust chemisorption with the formation of M―O<sub>ads</sub> bonds and intense electron transfer. Intriguingly, the adsorption energy presents a strong correlation with the <em>d</em>-band centers of the metal atoms. This finding is comprehended from the perspective of electron occupancy in antibonding orbitals in the adsorption systems. This work provides a feasible approach for modifying molecule adsorption on MSA-COF by regulating the <em>d</em>-band centers of metal atoms.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (95KB)</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 2407013"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145960","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":"Molten Intermediate Transportation-Oriented Synthesis of Amino-Rich g-C3N4 Nanosheets for Efficient Photocatalytic H2O2 Production","authors":"Guoqiang Chen , Zixuan Zheng , Wei Zhong , Guohong Wang , Xinhe Wu","doi":"10.3866/PKU.WHXB202406021","DOIUrl":"10.3866/PKU.WHXB202406021","url":null,"abstract":"<div><div>To eliminate the additional assistance of previously reported strategies for the synthesis of g-C<sub>3</sub>N<sub>4</sub> nanosheets such as templates, strong acids and alkalis, in this study, an innovative pattern for transportation of molten g-C<sub>3</sub>N<sub>4</sub> intermediates, without any additional substance assistance, has been resoundingly established to produce amino-rich g-C<sub>3</sub>N<sub>4</sub> nanosheets. The innovative pattern concretely contains the preliminary placement of melamine onto the top platform of an inverted crucible and their subsequent one-step calcination. During the calcination process, melamine and its subsequently formed g-C<sub>3</sub>N<sub>4</sub> intermediate can transform into a molten state and gradually stream down along the outer surface of inverted crucible. This molten intermediate transportation pattern contributes to remarkably resist severe aggregation, resulting in the final polymerization into amino-rich g-C<sub>3</sub>N<sub>4</sub> nanosheets in sequence. Moreover, the resultant amino-rich g-C<sub>3</sub>N<sub>4</sub> nanosheets exhibit an evidently enhanced photocatalytic H<sub>2</sub>O<sub>2</sub>-production rate of <em>ca.</em> 85.8 μmol·L<sup>–1</sup>·h<sup>–1</sup>, over 2 times superior to bulk g-C<sub>3</sub>N<sub>4</sub>, mainly due to the fact that in addition to their nanosheet structures with enhanced specific surface areas, their amino-rich structures can efficiently reinforce the adsorption of O<sub>2</sub> and *OOH intermediates to accelerate their effective transformation into H<sub>2</sub>O<sub>2</sub>. This work delivers an innovative pattern to synthesize amino-rich g-C<sub>3</sub>N<sub>4</sub> nanosheets with an insight into the photocatalytic mechanism.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (83KB)</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 2406021"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145017","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}
物理化学学报Pub Date : 2024-11-01DOI: 10.3866/PKU.WHXB202406020
Asif Hassan Raza, Shumail Farhan, Zhixian Yu, Yan Wu
{"title":"Double S-Scheme ZnS/ZnO/CdS Heterostructure Photocatalyst for Efficient Hydrogen Production","authors":"Asif Hassan Raza, Shumail Farhan, Zhixian Yu, Yan Wu","doi":"10.3866/PKU.WHXB202406020","DOIUrl":"10.3866/PKU.WHXB202406020","url":null,"abstract":"<div><div>This work illustrates the novelty of double S-scheme ZnS/ZnO/CdS ternary heterojunction photocatalyst with efficient photocatalytic activity. The sample with optimal CdS content, ZnS/ZnO/CdS-14% (ZZC14%), displayed the maximum H<sub>2</sub> evolution rate of 4.1 mmol·g<sup>‒1</sup>·h<sup>‒1</sup>. The maximum photocatalytic performance was approximately 2 and 13 times higher than their corresponding counterparts, ZnS/CdS and ZnO/ZnS, respectively. A high AQE of 19.8% under 420 nm was obtained. Additionally, the slight changes in H<sub>2</sub> evolution activities and retentions of crystal structures after six successive cycles indicate the stability of the photocatalyst. In accordance with the theoretical calculations and experimental results, the remarkable enhancement in photocatalytic activity is attributed to fast electron transfer and separation as well as the intimate contact due to mutual interaction between S-scheme. This work highlights an innovative approach to constructing a dual S-scheme photocatalytic system with high separation and fast migration capabilities of photogenerated charge carriers for splitting water to produce hydrogen.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (131KB)</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 2406020"},"PeriodicalIF":10.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143145961","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}