物理化学学报最新文献

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Work-function-engineered Mo 4d electronic structure modulation in Mo2C MXene cocatalyst for efficient photocatalytic H2 evolution 工作功能工程Mo2C MXene助催化剂中mo4d电子结构调制的高效光催化析氢
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-07-25 DOI: 10.1016/j.actphy.2025.100137
Ruiyun Liu , Ping Wang , Xuefei Wang , Feng Chen , Huogen Yu
{"title":"Work-function-engineered Mo 4d electronic structure modulation in Mo2C MXene cocatalyst for efficient photocatalytic H2 evolution","authors":"Ruiyun Liu ,&nbsp;Ping Wang ,&nbsp;Xuefei Wang ,&nbsp;Feng Chen ,&nbsp;Huogen Yu","doi":"10.1016/j.actphy.2025.100137","DOIUrl":"10.1016/j.actphy.2025.100137","url":null,"abstract":"<div><div>Mo<sub>2</sub>C MXene (Mo<sub>2</sub>CT<sub>x</sub>) exhibits exceptional hydrogen-evolution potential in photocatalysis due to the Pt-like electronic structure of surface Mo active sites. However, the Mo sites in Mo<sub>2</sub>CT<sub>x</sub> usually show excessively strong H-adsorption during HER, significantly limiting the intrinsic catalytic activity of Mo<sub>2</sub>CT<sub>x</sub>. To weaken the H-adsorption capacity of Mo active sites, a strategy of modulating <em>d</em>-orbital electron is implemented <em>via in-situ</em> constructing MoC-Mo<sub>2</sub>C MXene heterojunction by a work-function-induced effect. The MoC-Mo<sub>2</sub>CT<sub>x</sub> heterojunction was synthesized by <em>in</em><em>-</em><em>situ</em> conversion of Mo<sub>2</sub>C MXene into MoC <em>via</em> a Co-induced molten salt method, followed by coupling with TiO<sub>2</sub> through a simple ultrasonication-assisted method to prepare the MoC-Mo<sub>2</sub>CT<sub>x</sub>/TiO<sub>2</sub> photocatalyst. Photocatalytic tests showed that the optimal MoC-Mo<sub>2</sub>CT<sub>x</sub>/TiO<sub>2</sub> sample achieves an excellent hydrogen production rate of 1886 μmol h<sup>−1</sup> g<sup>−1</sup>, representing 117.9 and 3.9 fold enhancements over TiO<sub>2</sub> and Mo<sub>2</sub>CF<sub>x</sub>/TiO<sub>2</sub> (Mo<sub>2</sub>CF<sub>x</sub> prepared by a conventional etchant NH<sub>4</sub>F + HCl), respectively. Experimental and theoretical calculations substantiate that the work-function gradient between MoC and Mo<sub>2</sub>C MXene induces electron transfer from MoC to Mo<sub>2</sub>C MXene to weaken the H-adsorption of Mo active sites in Mo<sub>2</sub>CT<sub>x</sub> cocatalyst, thereby enhancing its HER activity. This research provides a new strategy of <em>in-situ</em> constructing Mo<sub>2</sub>C MXene-based heterojunction for adjusting the H-adsorption capacity of Mo active sites.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100137"},"PeriodicalIF":13.5,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144738530","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}
引用次数: 0
Waste medical mask-derived carbon quantum dots enhance the photocatalytic degradation of polyethylene terephthalate (PET) over BiOBr/g-C3N4 S-scheme heterojunction 废弃医用掩膜衍生的碳量子点在BiOBr/g-C3N4 S-scheme异质结上增强了对聚对苯二甲酸乙二醇酯(PET)的光催化降解
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-07-25 DOI: 10.1016/j.actphy.2025.100135
Shiyi Chen, Jialong Fu, Jianping Qiu, Guoju Chang, Shiyou Hao
{"title":"Waste medical mask-derived carbon quantum dots enhance the photocatalytic degradation of polyethylene terephthalate (PET) over BiOBr/g-C3N4 S-scheme heterojunction","authors":"Shiyi Chen,&nbsp;Jialong Fu,&nbsp;Jianping Qiu,&nbsp;Guoju Chang,&nbsp;Shiyou Hao","doi":"10.1016/j.actphy.2025.100135","DOIUrl":"10.1016/j.actphy.2025.100135","url":null,"abstract":"<div><div>The coronavirus disease 2019 (COVID-19) pandemic has increased the necessity of medical masks, and to date, many waste masks have been discarded without being reprocessed, causing environmental harm. PET, a commonly used plastic product, presents certain hurdles to its natural degradation. In this work, waste medical masks were converted into carbon quantum dots (MCQDs) with blue fluorescence emissions using a simple solvothermal process and then doped into BiOBr/g-C<sub>3</sub>N<sub>4</sub> composite material to construct S-scheme heterojunctions for PET degradation. Density functional theory (DFT) calculations revealed that an interfacial electric field (IEF) was formed between g-C<sub>3</sub>N<sub>4</sub> and BiOBr. The findings demonstrate that the MCQDs, as a cocatalyst for electron transmission and storage, encourage S-scheme heterojunctions to further separate photogenerated electrons and holes. Levofloxacin (LEV) was used as a molecular probe to visually compare the catalytic activities of various catalysts. These catalysts with different photocatalytic activity were then used to degrade PET. The findings demonstrate that the degradation efficiency of PET over the BiOBr/g-C<sub>3</sub>N<sub>4</sub>/3MCQDs in seawater is 39.88 ± 1.04 % (weight loss), which is 1.37 times higher than that of BiOBr/g-C<sub>3</sub>N<sub>4</sub>, and also better than those reported in most of the literature. Free radical capture tests, electrostatic field orbital trap high-resolution gas chromatography-mass spectrometry (HRGC-MS), and ultra-performance liquid chromatography-mass spectrometry (UPLC-MS) experiments uncovered and briefly revealed the key products in the photocatalytic degradation of PET, as well as the relevant mechanism of photocatalytic degradation of PET. The degradation products are expected to become precursors for the further production of polymers and medicines, <em>etc</em>. This study offers fresh perspectives for the creation of innovative photocatalysts for the ecologically benign breakdown of PET, which helps to further lessen environmental damage caused by microplastics (MPs) and enhance resource sustainability.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100135"},"PeriodicalIF":13.5,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195915","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}
引用次数: 0
Ultrafast electron transfer at the ZIS1−x/UCN S-scheme interface enables efficient H2O2 photosynthesis coupled with tetracycline degradation ZIS1−x/UCN S-scheme界面的超快电子转移实现了高效的H2O2光合作用和四环素降解
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-07-24 DOI: 10.1016/j.actphy.2025.100136
Shumin Zhang , Yaqi Wang , Zelin Wang , Libo Wang , Changsheng An , Difa Xu
{"title":"Ultrafast electron transfer at the ZIS1−x/UCN S-scheme interface enables efficient H2O2 photosynthesis coupled with tetracycline degradation","authors":"Shumin Zhang ,&nbsp;Yaqi Wang ,&nbsp;Zelin Wang ,&nbsp;Libo Wang ,&nbsp;Changsheng An ,&nbsp;Difa Xu","doi":"10.1016/j.actphy.2025.100136","DOIUrl":"10.1016/j.actphy.2025.100136","url":null,"abstract":"<div><div>Coupling H<sub>2</sub>O<sub>2</sub> production with organic pollutant degradation can effectively overcome the sluggish kinetics of water oxidation while concurrently addressing environmental pollution challenges. In this work, an S-defect-rich ZnIn<sub>2</sub>S<sub>4</sub>/g-C<sub>3</sub>N<sub>4</sub> (ZIS<sub>1−<em>x</em></sub>/UCN) S-scheme heterojunction photocatalyst was constructed by <em>in situ</em> growing ZIS<sub>1−<em>x</em></sub> nanosheets on porous ultrathin UCN. The designed ZIS<sub>1−<em>x</em></sub>/UCN photocatalyst demonstrates enhanced visible light absorption, abundant active sites, and intimate interfacial contact. The optimized ZIS<sub>1−<em>x</em></sub>/UCN-1.0 photocatalyst exhibits outstanding dual functionality, simultaneously achieving an H<sub>2</sub>O<sub>2</sub> production rate of 2902.2 μmol g<sup>−1</sup> h<sup>−1</sup> and 91.3 % tetracycline (50 mg L<sup>−1</sup>) degradation efficiency. This H<sub>2</sub>O<sub>2</sub> performance represents a 1.63-fold enhancement compared to its activity in pure water (1777.0 μmol g<sup>−1</sup> h<sup>−1</sup>). Through comprehensive characterization including femtosecond transient absorption spectroscopy (fs-TAS), <em>in situ</em> irradiation X-ray photoelectron spectroscopy (ISI-XPS), and <em>in situ</em> X-ray absorption fine structure spectroscopy (XAFS), we unequivocally confirm the S-scheme charge transfer mechanism. This S-scheme induced unique electronic structure not only fosters ultrafast electron transfer at the interface (3.54 ps) but also significantly enhances the redox capacity of photogenerated carriers. Collectively, this work opens new avenues for the dual application of photocatalytic technology in both energy production and environmental remediation.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100136"},"PeriodicalIF":13.5,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720990","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}
引用次数: 0
Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO2 hydrogenation 分子筛催化氧化铟催化剂增强光催化CO2加氢作用
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-07-22 DOI: 10.1016/j.actphy.2025.100133
Qinhui Guan , Yuhao Guo , Na Li , Jing Li , Tingjiang Yan
{"title":"Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO2 hydrogenation","authors":"Qinhui Guan ,&nbsp;Yuhao Guo ,&nbsp;Na Li ,&nbsp;Jing Li ,&nbsp;Tingjiang Yan","doi":"10.1016/j.actphy.2025.100133","DOIUrl":"10.1016/j.actphy.2025.100133","url":null,"abstract":"<div><div>In the realm of photocatalytic CO<sub>2</sub> hydrogenation, the adsorption-desorption behaviors and dynamics of photogenerated carriers are pivotal determinants of the kinetic processes and overall efficiency of photocatalytic reactions. Herein, 5A molecular sieve-functionalized In<sub>2</sub>O<sub>3</sub> composites (denoted as IO@5A-<em>x</em>wt%) were fabricated through a facile impregnation-calcination method. Among them, the IO@5A-5wt% composite, with the optimized loading amount of 5A molecular sieves, showcases outstanding performance in photocatalytic conversion of CO<sub>2</sub> to CO, achieving a CO production rate of 2610.55 μmol g<sup>−1</sup> h<sup>−1</sup>, which is 19 times higher than that of pristine In<sub>2</sub>O<sub>3</sub>. Moreover, the IO@5A-5wt% composite maintains acceptable catalytic stability after a prolonged experiment lasting 45 h and total of 108 cycles. A comprehensive series of characterization techniques and performance evaluations reveal that the incorporation of 5A molecular sieves significantly modulates the adsorption-desorption behavior and hole dynamics during photocatalytic reactions. The multi-channel architecture of 5A molecular sieves, featuring suitable pore sizes, effectively enhances CO<sub>2</sub> adsorption. Meanwhile, the surface hydroxyl groups of 5A molecular sieves facilitate the transfer of photogenerated holes, thereby suppressing the recombination of photogenerated carriers. Additionally, the reaction product H<sub>2</sub>O desorbs more readily from the catalyst surface. These synergistic effects collectively constitute the key mechanism underlying the enhanced photocatalytic performance of the IO@5A-5wt% composite.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100133"},"PeriodicalIF":13.5,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144749480","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}
引用次数: 0
3D/2D ReSe2/ZnCdS S-scheme photocatalyst with efficient interfacial charge separation for optimized hydrogen production 具有高效界面电荷分离的3D/2D ReSe2/ZnCdS S-scheme光催化剂优化制氢
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-07-18 DOI: 10.1016/j.actphy.2025.100131
Jiaqi Yang , Xuqiang Hao , Jiejie Jing , Yuqiang Hao , Zhiliang Jin
{"title":"3D/2D ReSe2/ZnCdS S-scheme photocatalyst with efficient interfacial charge separation for optimized hydrogen production","authors":"Jiaqi Yang ,&nbsp;Xuqiang Hao ,&nbsp;Jiejie Jing ,&nbsp;Yuqiang Hao ,&nbsp;Zhiliang Jin","doi":"10.1016/j.actphy.2025.100131","DOIUrl":"10.1016/j.actphy.2025.100131","url":null,"abstract":"<div><div>The rational construction of step-scheme (S-scheme) heterojunctions has been demonstrated as an effective strategy to optimize interfacial charge carrier separation dynamics in semiconductor photocatalysts. In this work, a hierarchical ReSe<sub>2</sub>/ZnCdS S-scheme heterojunction with well-defined architectures was successfully synthesized <em>via</em> an ultrasonication-assisted synthetic strategy, achieving precise nanostructure control and enhanced interfacial coupling for optimized photogenerated charge dynamics. The disordered nanoflower-like ReSe<sub>2</sub> architecture enhances light-harvesting efficiency and the density of surface reaction sites, and significantly suppresses ZnCdS nanoparticle aggregation. The optimized 5 % ReSe<sub>2</sub>/ZnCdS composite exhibits an exceptional hydrogen evolution rate of 13.96 mmol g<sup>−1</sup> h<sup>−1</sup> under visible light irradiation, representing a 5.91-fold enhancement over pristine ZnCdS (2.36 mmol g<sup>−1</sup> h<sup>−1</sup>) and outperforming most conventional heterojunction systems. The outstanding photocatalytic performance is attributed to the formation of the ReSe<sub>2</sub>/ZnCdS S-scheme heterojunction, which promotes the separation of photogenerated electrons and holes, enhancing the photo-redox capacity. Combining <em>in-situ</em> XPS analysis and DFT calculations further conforms the S-scheme charge transfer mechanism at the heterointerface of ReSe<sub>2</sub>/ZnCdS. Furthermore, Gibbs free energy calculations of hydrogen adsorption confirm that ReSe<sub>2</sub> as the predominant catalytic center provides more favorable hydrogen adsorption kinetics than ZnCdS. This work provides a universal framework to design ZnCdS-based S-scheme heterojunctions for high-efficiency photocatalytic hydrogen evolution.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100131"},"PeriodicalIF":10.8,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144694605","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}
引用次数: 0
Synergistic Carbon Doping and Cu Loading on Boron Nitride via Microwave Synthesis for Enhanced Atmospheric CO2 Photoreduction 微波合成氮化硼协同碳掺杂和Cu负载增强大气CO2光还原
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-07-18 DOI: 10.1016/j.actphy.2025.100132
Haotong Ma , Mingyu Heng , Yang Xu , Wei Bi , Yingchun Miao , Shuning Xiao
{"title":"Synergistic Carbon Doping and Cu Loading on Boron Nitride via Microwave Synthesis for Enhanced Atmospheric CO2 Photoreduction","authors":"Haotong Ma ,&nbsp;Mingyu Heng ,&nbsp;Yang Xu ,&nbsp;Wei Bi ,&nbsp;Yingchun Miao ,&nbsp;Shuning Xiao","doi":"10.1016/j.actphy.2025.100132","DOIUrl":"10.1016/j.actphy.2025.100132","url":null,"abstract":"<div><div>Photocatalytic CO<sub>2</sub> reduction under atmospheric concentrations remains highly challenging yet critical for practical carbon-neutral applications. In this study, a Cu-loaded, carbon-doped boron nitride (Cu/BCN) photocatalyst was synthesized by a microwave-assisted molten salt method. This approach enables simultaneous carbon incorporation into the BN lattice and selective deposition of Cu nanoparticles, forming an efficient heterostructure. The synergy between C doping and Cu loading modulates the band structure, enhances visible-light absorption, promotes charge separation, and improves CO<sub>2</sub> adsorption. The optimized Cu/BCN photocatalyst achieved a CO production rate of 30.62 μmol g<sup>−1</sup> h<sup>−1</sup> with 95.8 % selectivity under ambient CO<sub>2</sub> conditions. Combined experimental and DFT analyses confirm that the Cu/BCN interface facilitates charge transfer and lowers the energy barrier for ∗COOH formation. This work demonstrates a promising route toward efficient CO<sub>2</sub> utilization directly from air, offering a scalable strategy for atmospheric carbon conversion.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100132"},"PeriodicalIF":10.8,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144694549","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}
引用次数: 0
Ga-doped Cu/γ-Al2O3 bifunctional interface sites promote the direct hydrogenation of CO2 to DME ga掺杂Cu/γ-Al2O3双功能界面位点促进CO2直接加氢生成二甲醚
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-28 DOI: 10.1016/j.actphy.2025.100126
Xiaorui Chen , Xuan Luo , Tongming Su , Xinling Xie , Liuyun Chen , Yuejing Bin , Zuzeng Qin , Hongbing Ji
{"title":"Ga-doped Cu/γ-Al2O3 bifunctional interface sites promote the direct hydrogenation of CO2 to DME","authors":"Xiaorui Chen ,&nbsp;Xuan Luo ,&nbsp;Tongming Su ,&nbsp;Xinling Xie ,&nbsp;Liuyun Chen ,&nbsp;Yuejing Bin ,&nbsp;Zuzeng Qin ,&nbsp;Hongbing Ji","doi":"10.1016/j.actphy.2025.100126","DOIUrl":"10.1016/j.actphy.2025.100126","url":null,"abstract":"<div><div>The reaction of CO<sub>2</sub> catalytic hydrogenation to dimethyl ether (DME) usually relies on a Cu-containing metal oxide/molecular sieve system; however, the migration of copper species to molecular sieves is unavoidable during the reaction, leading to the loss of Cu<sup>0</sup> sites and acidic sites. In this work, a Cu/<em>x</em>%Ga-γ-Al<sub>2</sub>O<sub>3</sub> bifunctional catalyst was synthesized <em>via</em> the coprecipitation method. Ga was doped into the γ-Al<sub>2</sub>O<sub>3</sub> lattice at a low concentration, forming interfacial active sites with surface Cu<sup>0</sup> species to achieve the hydrogenation of CO<sub>2</sub> to DME. Experimental studies combined with DFT calculations demonstrate that the catalyst remains stable for 180 h and that the Ga-doped Cu/γ-Al<sub>2</sub>O<sub>3</sub> interface sites exhibit catalytic effects on CO<sub>2</sub> hydrogenation to CH<sub>3</sub>OH and CH<sub>3</sub>OH dehydration to produce DME. The doping of Ga increases the specific surface area of the catalyst, reduces the particle size of Cu<sup>0</sup>, enhances the number of acidic and basic sites on the catalyst, and promotes the adsorption of H<sub>2</sub> and CO<sub>2</sub>. In addition, a new reaction pathway for DME synthesis was proposed. This work removes the dehydrated component of a traditional Cu-based bifunctional catalyst, enabling two reactions to occur at the same active sites, thus providing a new strategy for the design of novel dimethyl ether synthesis bifunctional catalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100126"},"PeriodicalIF":10.8,"publicationDate":"2025-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535388","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}
引用次数: 0
MOF-derived ZnO/PANI S-scheme heterojunction for efficient photocatalytic phenol mineralization coupled with H2O2 generation mof衍生的ZnO/PANI s型异质结用于光催化苯酚矿化和H2O2生成
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-17 DOI: 10.1016/j.actphy.2025.100121
Bowen Liu , Jianjun Zhang , Han Li , Bei Cheng , Chuanbiao Bie
{"title":"MOF-derived ZnO/PANI S-scheme heterojunction for efficient photocatalytic phenol mineralization coupled with H2O2 generation","authors":"Bowen Liu ,&nbsp;Jianjun Zhang ,&nbsp;Han Li ,&nbsp;Bei Cheng ,&nbsp;Chuanbiao Bie","doi":"10.1016/j.actphy.2025.100121","DOIUrl":"10.1016/j.actphy.2025.100121","url":null,"abstract":"<div><div>Complete mineralization of persistent organic pollutants in wastewater remains a formidable challenge. Here, we report the rational design of a ZIF-8-derived ZnO/polyaniline (PANI) S-scheme heterojunction synthesized <em>via in situ</em> oxidative polymerization. Advanced characterizations confirm the S-scheme charge transfer mechanism within the ZnO/PANI heterojunction. The optimized composite achieves complete phenol mineralization within 60 min while concurrently generating H<sub>2</sub>O<sub>2</sub> at a rate of 0.75 mmol∙L<sup>−1</sup>·h<sup>−1</sup> under simulated solar irradiation. Mechanistic studies verify that the S-scheme heterojunction retains strong redox potentials, driving the formation of reactive oxygen species for H<sub>2</sub>O<sub>2</sub> production and phenol degradation. This work establishes a universal design paradigm for MOF-derived inorganic/organic S-scheme heterojunctions, effectively coupling solar-driven energy conversion with environmental remediation.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100121"},"PeriodicalIF":10.8,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144330018","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}
引用次数: 0
BiVO4/WO3−x S-scheme heterojunctions with amplified internal electric field for boosting photothermal-catalytic activity 具有放大内电场的BiVO4/WO3−x s方案异质结提高光热催化活性
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-17 DOI: 10.1016/j.actphy.2025.100122
Ziyang Long , Quanzheng Li , Chengliang Zhang , Haifeng Shi
{"title":"BiVO4/WO3−x S-scheme heterojunctions with amplified internal electric field for boosting photothermal-catalytic activity","authors":"Ziyang Long ,&nbsp;Quanzheng Li ,&nbsp;Chengliang Zhang ,&nbsp;Haifeng Shi","doi":"10.1016/j.actphy.2025.100122","DOIUrl":"10.1016/j.actphy.2025.100122","url":null,"abstract":"<div><div>Modulating the internal electric field (IEF) remains a critical challenge for S-scheme heterojunction photocatalysts. The BiVO<sub>4</sub>/WO<sub>3−<em>x</em></sub> S-scheme heterojunctions were successfully prepared to purify the wastewater environment where TC and Cr (VI) coexist under visible light illumination. The BiVO<sub>4</sub>/WO<sub>3−<em>x</em></sub> with 10 wt% WO<sub>3−<em>x</em></sub> (BVO/WO<sub>3−<em>x</em></sub>-10) demonstrated superior photocatalytic efficiency, which could degrade 78.5 % of TC and reduce 85.3 % of Cr(VI) in 60 min. The photocatalytic activity of BVO/WO<sub>3−<em>x</em></sub>−10 displayed enhanced removal efficiency in the mixed system. The removal ability of TC and Cr (Ⅵ) was increased by 1.29 and 1.32 times, respectively. Based on IR thermography measurements, the elevated reaction system temperatures were ascribed to the photothermal effect of WO<sub>3−<em>x</em></sub>. Oxygen vacancies (OVs) could amplify the energy band difference between WO<sub>3−<em>x</em></sub> and BiVO<sub>4</sub>, which strengthens the IEF and accelerates the separation of carriers. A detailed degradation pathway and intermediate toxicity were carried out using the mung bean experiment and the results of the LC−MS. In general, this work provided new insights for regulating IEF to enhance the degradation efficiency in mixed wastewater and the carriers separation in the S-scheme heterojunction of the photothermal-catalytic system.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100122"},"PeriodicalIF":10.8,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144330019","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}
引用次数: 0
Catalysts for electrocatalytic dechlorination of chlorinated aromatic hydrocarbons: synthetic strategies, applications, and challenges 电催化氯化芳烃脱氯催化剂:合成策略、应用和挑战
IF 10.8 2区 化学
物理化学学报 Pub Date : 2025-06-14 DOI: 10.1016/j.actphy.2025.100120
Qi Wang , Yuqing Liu , Jiefei Wang , Yuan-Yuan Ma , Jing Du , Zhan-Gang Han
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