物理化学学报最新文献

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SBA-15 templated covalent triazine frameworks for boosted photocatalytic hydrogen production SBA-15模板化共价三嗪框架促进光催化制氢
IF 13.5 2区 化学
物理化学学报 Pub Date : 2026-01-01 Epub Date: 2025-08-08 DOI: 10.1016/j.actphy.2025.100149
Chengxiao Zhao , Zhaolin Li , Dongfang Wu , Xiaofei Yang
{"title":"SBA-15 templated covalent triazine frameworks for boosted photocatalytic hydrogen production","authors":"Chengxiao Zhao ,&nbsp;Zhaolin Li ,&nbsp;Dongfang Wu ,&nbsp;Xiaofei Yang","doi":"10.1016/j.actphy.2025.100149","DOIUrl":"10.1016/j.actphy.2025.100149","url":null,"abstract":"<div><div>Covalent triazine frameworks (CTFs) represent an attractive family of metal-free visible light-responsive covalent organic frameworks (COFs), possessing promising characteristics such as large specific surface area, rich nitrogen content, permanent porosity, and high thermal and chemical stability for photocatalytic hydrogen production via water splitting. Nevertheless, the majority of CTFs are confronted with difficulty in chemical synthesis and generally suffer from low electric conductivity and severe photogenerated charge carrier recombination during photocatalytic hydrogen evolution reaction (HER). The hydrogen-evolving performance highly depends on the structure of <em>π</em>-conjugated CTFs and the synthetic methods, and controlled synthesis of well-defined nanostructures is still highly challenging. In this work, we report the organic acid-catalyzed synthesis of porous CTF nanoarchitectures templated by mesoporous silica molecular sieve SBA-15 with a highly ordered hexagonal structure. The SBA-15 templated CTF-S2 nanorods exhibited a substantial increase in photocatalytic HER efficiency, with an impressive 14-fold enhancement compared to the micro-sized bulk CTF-1 (4.1 μmol h<sup>−1</sup>). This remarkable improvement in the photocatalytic HER over SBA-templated CTF-S2 nanostructure is attributed to the extended visible light absorption, accelerated charge carrier transfer and the optimized band structure.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100149"},"PeriodicalIF":13.5,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195917","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 : 2026-01-01 Epub 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":"2026-01-01","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
Modulate surface potential well depth of Bi12O17Cl2 by FeOOH in Bi12O17Cl2@FeOOH heterojunction to boost piezoelectric charge transfer and piezo-self-Fenton catalysis FeOOH在Bi12O17Cl2@FeOOH异质结中调制Bi12O17Cl2表面电位井深,促进压电电荷转移和压电自fenton催化
IF 13.5 2区 化学
物理化学学报 Pub Date : 2026-01-01 Epub Date: 2025-08-13 DOI: 10.1016/j.actphy.2025.100157
Jiangyuan Qiu , Tao Yu , Junxin Chen , Wenxuan Li , Xiaoxuan Zhang , Jinsheng Li , Rui Guo , Zaiyin Huang , Xuanwen Liu
{"title":"Modulate surface potential well depth of Bi12O17Cl2 by FeOOH in Bi12O17Cl2@FeOOH heterojunction to boost piezoelectric charge transfer and piezo-self-Fenton catalysis","authors":"Jiangyuan Qiu ,&nbsp;Tao Yu ,&nbsp;Junxin Chen ,&nbsp;Wenxuan Li ,&nbsp;Xiaoxuan Zhang ,&nbsp;Jinsheng Li ,&nbsp;Rui Guo ,&nbsp;Zaiyin Huang ,&nbsp;Xuanwen Liu","doi":"10.1016/j.actphy.2025.100157","DOIUrl":"10.1016/j.actphy.2025.100157","url":null,"abstract":"<div><div>Although the design of heterojunction piezoelectric catalysts has significantly enhanced catalytic activity, the regulatory mechanisms of heterojunction interfaces on surface potential wells during piezoelectric processes and their impact on carrier migration still lack systematic investigation. This work constructs an enhance interface interaction heterointerface between amorphous FeOOH and Bi<sub>12</sub>O<sub>17</sub>Cl<sub>2</sub> (BOC) in Bi<sub>12</sub>O<sub>17</sub>Cl<sub>2</sub>@FeOOH through a self-assembly strategy. This strong interfacial interaction significantly enhances interface polarity can substantially suppress the stress-responsive capability of surface charges on BOC (maximum reduction reached as high as 63 %–98 % of original value). This significantly reduces the depth of surface potential wells during piezoelectric processes, thereby effectively weakening piezoelectric charge confinement while promoting charge transfer. Concurrently, Bi–O–Fe chemical bonds formed at the interface and establish charge transport channels. These synergistic mechanisms elevate the H<sub>2</sub>O<sub>2</sub> production rate to 3.04 mmol g<sup>−1</sup> h<sup>−1</sup> for participate in the piezoelectric self-Fenton reaction and the removal rate of total organic carbon increased 3 fold (18.6 % <em>vs</em> 55.8 %).</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100157"},"PeriodicalIF":13.5,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145264484","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
Ionic-bond crosslinked carbonized polymer dots for tunable and enhanced room temperature phosphorescence 可调和增强室温磷光的离子键交联碳化聚合物点
IF 13.5 2区 化学
物理化学学报 Pub Date : 2026-01-01 Epub Date: 2025-08-11 DOI: 10.1016/j.actphy.2025.100156
Chunyuan Kang , Xiaoyu Li , Fan Yang, Bai Yang
{"title":"Ionic-bond crosslinked carbonized polymer dots for tunable and enhanced room temperature phosphorescence","authors":"Chunyuan Kang ,&nbsp;Xiaoyu Li ,&nbsp;Fan Yang,&nbsp;Bai Yang","doi":"10.1016/j.actphy.2025.100156","DOIUrl":"10.1016/j.actphy.2025.100156","url":null,"abstract":"<div><div>Carbonized polymer dots (CPDs) have emerged as promising room temperature phosphorescent (RTP) materials owing to their tunable luminescence and facile synthesis. However, current strategies relying on hydrogen/covalent bond for luminescence enhancement suffer from limited phosphorescence intensity, and color diversity (primarily green). This work proposes constructing ionic-bond crosslinked network as a novel design strategy to address these limitations. Owing to the high strength, non-directionality and non-saturation of ionic bond, crosslinked networks are constructed to immobilize chromophores and suppress non-radiative transitions. By incorporating lithium ions into poly(acrylic acid)-based CPDs, the photoluminescence quantum yield is dramatically enhanced from 1.1 % to 48.4 %, with a 40-fold increase in phosphorescence intensity. Further introduction of zinc ions enables tunable RTP emission from green to yellow via transition metal doping. This strategy achieves effective regulation of RTP intensity and wavelength in CPDs, providing a versatile platform for designing advanced organic phosphorescent materials with tailored RTP properties.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100156"},"PeriodicalIF":13.5,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145264485","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 design of high-entropy P2/O3 biphasic cathodes for high-performance sodium-ion batteries 高性能钠离子电池用高熵P2/O3双相阴极协同设计
IF 13.5 2区 化学
物理化学学报 Pub Date : 2026-01-01 Epub Date: 2025-07-09 DOI: 10.1016/j.actphy.2025.100129
Shan Zhao , Xu Liu , Haotian Guo , Zonglin Liu , Pengfei Wang , Jie Shu , Tingfeng Yi
{"title":"Synergistic design of high-entropy P2/O3 biphasic cathodes for high-performance sodium-ion batteries","authors":"Shan Zhao ,&nbsp;Xu Liu ,&nbsp;Haotian Guo ,&nbsp;Zonglin Liu ,&nbsp;Pengfei Wang ,&nbsp;Jie Shu ,&nbsp;Tingfeng Yi","doi":"10.1016/j.actphy.2025.100129","DOIUrl":"10.1016/j.actphy.2025.100129","url":null,"abstract":"&lt;div&gt;&lt;div&gt;P2-type layered transition metal oxides (P2-Na&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt;TMO&lt;sub&gt;2&lt;/sub&gt;) have emerged as promising cathodes for sodium-ion batteries (SIBs) owing to their superior cycling stability and excellent rate capability. However, their practical application is significantly hindered by two major challenges. Firstly, irreversible phase transitions occur during high-voltage operation, which disrupt the structural integrity and deteriorate electrochemical performance. Secondly, their inherently low theoretical specific capacity fails to meet modern energy demands. To tackle these challenges, this study proposes a novel synergistic strategy that integrates high-entropy engineering with a biphasic P2/O3 structural design. An innovative cathode material, Na&lt;sub&gt;0.70&lt;/sub&gt;Ni&lt;sub&gt;0.25&lt;/sub&gt;Mn&lt;sub&gt;0.35&lt;/sub&gt;Co&lt;sub&gt;0.15&lt;/sub&gt;Fe&lt;sub&gt;0.05&lt;/sub&gt;Ti&lt;sub&gt;0.20&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; (denoted as Na&lt;sub&gt;0.70&lt;/sub&gt;NMCFT), was successfully synthesized via a high-temperature solid-state reaction. This material design critically incorporates five distinct transition metal cations into the transition metal (TM) layer, constructing a stabilized high-entropy configuration. Careful optimization of both the five TM elements and the sodium content was essential to precisely regulate the synthesis and formation of the desired integrated P2/O3 biphasic structure within this high-entropy host. Comprehensive structural characterization unequivocally confirms the successful construction of this tailored architecture. X-ray diffraction (XRD) and transmission electron microscopy (TEM) collectively confirm the successful construction of the P2/O3 biphasic architecture. The high-entropy engineering stabilizes the P2 phase through configurational entropy, effectively suppressing irreversible phase transitions and Na&lt;sup&gt;+&lt;/sup&gt;/vacancy ordering during cycling, as evidenced by smoother charge/discharge profiles and &lt;em&gt;ex-situ&lt;/em&gt; XRD analysis under high potentials. Meanwhile, the introduced O3 phase compensates for capacity shortages and improves cycling stability, working in tandem with the P2 phase. Critically, the interaction between the two phases enables a highly reversible transition between P2/O3-P2/P3, further enhancing the overall performance. Under the combined action of the high-entropy and biphasic strategies, Na&lt;sub&gt;0.70&lt;/sub&gt;NMCFT exhibits optimal electrochemical performance. It delivers an initial discharge capacity of 102.08 mAh∙g&lt;sup&gt;−1&lt;/sup&gt; at 1&lt;em&gt;C&lt;/em&gt;, retaining 88.15 % after 200 cycles, demonstrating exceptional cycling stability. Moreover, even at 10&lt;em&gt;C&lt;/em&gt;, Na&lt;sub&gt;0.70&lt;/sub&gt;NMCFT still has an initial discharge specific capacity of 85.67 mAh∙g&lt;sup&gt;−1&lt;/sup&gt; and a capacity retention of up to 70 % after 1000 cycles. Kinetic analyses further reveal that Na&lt;sub&gt;0.70&lt;/sub&gt;NMCFT possesses the lowest charge transfer resistance and the highest sodium-ion diffusion coefficient among the materials studied. In conclusion, this work demonstrates that the ratio","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 1","pages":"Article 100129"},"PeriodicalIF":13.5,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145334186","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
Constructing S-scheme heterojunctions by integrating covalent organic frameworks with transition metal sulfides for efficient noble-metal-free photocatalytic hydrogen evolution 通过将共价有机框架与过渡金属硫化物集成构建s型异质结,实现高效的无贵金属光催化析氢
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-12-01 Epub Date: 2025-08-14 DOI: 10.1016/j.actphy.2025.100152
Xinwan Zhao , Yue Cao , Minjun Lei , Zhiliang Jin , Noritatsu Tsubaki
{"title":"Constructing S-scheme heterojunctions by integrating covalent organic frameworks with transition metal sulfides for efficient noble-metal-free photocatalytic hydrogen evolution","authors":"Xinwan Zhao ,&nbsp;Yue Cao ,&nbsp;Minjun Lei ,&nbsp;Zhiliang Jin ,&nbsp;Noritatsu Tsubaki","doi":"10.1016/j.actphy.2025.100152","DOIUrl":"10.1016/j.actphy.2025.100152","url":null,"abstract":"<div><div>Two-dimensional covalent organic frameworks (COFs) are considered among the most potential crystalline porous materials for solar-driven hydrogen production. However, it is usually necessary to introduce noble metal cocatalysts to boost the hydrogen evolution capacity of COFs. In this work, a unique S-scheme heterojunction structured TtTfp-COF/NiS composite material was effectively developed by growing metal sulfide on the typical two-dimensional covalent organic framework TtTfp-COF through a simple solvothermal synthesis method. In this structure, linear structure of rod-like NiS is more stable and convenient for further surface modification. It also provides key active sites and promotes efficient electron transfer, significantly enhancing the hydrogen evolution efficiency. The covalent organic framework enhances charge carrier transport efficiency by controlling the spatial organization of precursors and ligands. It is indicated by the experimental findings that a hydrogen evolution rate of 5978 μmol g<sup>−1</sup> h<sup>−1</sup> can be achieved for the NT-20 sample, which about 11.5 times higher than that of the initial TtTfp-COF (520 μmol g<sup>−1</sup> h<sup>−1</sup>). In addition, the material exhibits a notable quantum efficiency of 1.96 % when exposed to 420 nm illumination. Both experimental results and theoretical analyses have been confirmed to improve the hydrogen evolution rate <em>via</em> photocatalysis and the charge transfer mechanism within the S-scheme heterojunction has been thoroughly elucidated. The design and development of non-precious metal COF-based photocatalysts are provided with new insights in this article, and new ideas for the construction of S-scheme heterojunctions are offered by the synergistic combination of inorganic and organic materials in photocatalysis.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 12","pages":"Article 100152"},"PeriodicalIF":13.5,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144894773","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
Understanding the effect of pH on protonated COF during photocatalytic H2O2 production by femtosecond transient absorption spectroscopy 用飞秒瞬态吸收光谱法研究光催化生产H2O2过程中pH对质子化COF的影响
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-12-01 Epub Date: 2025-08-15 DOI: 10.1016/j.actphy.2025.100160
Xin Zhou , Yiting Huo , Songyu Yang , Bowen He , Xiaojing Wang , Zhen Wu , Jianjun Zhang
{"title":"Understanding the effect of pH on protonated COF during photocatalytic H2O2 production by femtosecond transient absorption spectroscopy","authors":"Xin Zhou ,&nbsp;Yiting Huo ,&nbsp;Songyu Yang ,&nbsp;Bowen He ,&nbsp;Xiaojing Wang ,&nbsp;Zhen Wu ,&nbsp;Jianjun Zhang","doi":"10.1016/j.actphy.2025.100160","DOIUrl":"10.1016/j.actphy.2025.100160","url":null,"abstract":"<div><div>Covalent organic frameworks (COFs), recognized for their precisely tunable microstructures and high surface area, are promising photocatalysts for hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production. However, the critical influence of pH on the stability of COF during the photocatalytic H<sub>2</sub>O<sub>2</sub> production remains poorly understood. In this work, the photocatalytic H<sub>2</sub>O<sub>2</sub> production performance of an imine-linked COF is significantly enhanced through a simple protonation strategy. Crucially, the protonated COF exhibits excellent stability under weakly acidic conditions (pH ≥ 3), but undergoes irreversible hydrolyzed under strongly acidic conditions (pH &lt; 3). The protonation occurs specifically at the nitrogen atoms of imine units and serves a dual function: it suppresses ultrafast charge recombination (as revealed by femtosecond transient absorption spectroscopy) and directly provides a proton source for H<sub>2</sub>O<sub>2</sub> generation. Moreover, fluoride ions (F<sup>−</sup>) are introduced into the photocatalytic system to further improve the photocatalytic H<sub>2</sub>O<sub>2</sub> production rate. The strong electronegativity of F<sup>−</sup> facilitates electron transfer from COF to F<sup>−</sup>, thus realizing the spatial separation of photogenerated carriers. Mechanistic studies confirm that H<sub>2</sub>O<sub>2</sub> production follows a two-electron oxygen reduction reaction pathway. These findings elucidate the pH-dependent stability and activity of protonated COFs, provide fundamental insights into charge carrier dynamics, and establishe design principles to develop highly efficient and stable COF-based photocatalysts for solar-driven H<sub>2</sub>O<sub>2</sub> generation.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 12","pages":"Article 100160"},"PeriodicalIF":13.5,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144907852","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
Ni-induced modulation of Pt 5d–H 1s antibonding orbitals for enhanced hydrogen evolution and urea oxidation 镍诱导的Pt 5d-H - 1s反键轨道的调制促进了析氢和尿素氧化
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-12-01 Epub Date: 2025-08-14 DOI: 10.1016/j.actphy.2025.100159
Ruyan Liu , Zhenrui Ni , Olim Ruzimuradov , Khayit Turayev , Tao Liu , Luo Yu , Panyong Kuang
{"title":"Ni-induced modulation of Pt 5d–H 1s antibonding orbitals for enhanced hydrogen evolution and urea oxidation","authors":"Ruyan Liu ,&nbsp;Zhenrui Ni ,&nbsp;Olim Ruzimuradov ,&nbsp;Khayit Turayev ,&nbsp;Tao Liu ,&nbsp;Luo Yu ,&nbsp;Panyong Kuang","doi":"10.1016/j.actphy.2025.100159","DOIUrl":"10.1016/j.actphy.2025.100159","url":null,"abstract":"<div><div>While H<sub>2</sub> features high energy density, environmental friendliness, and renewability, its efficient production is limited by the sluggish kinetics of the oxygen evolution reaction (OER). Here, we report a Pt@PtNi<sub>3</sub> core@shell alloy electrocatalyst that, through Ni incorporation, modulates the occupancy of Pt 5<em>d</em> antibonding orbitals and simultaneously enhances both hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) activities. The optimized Pt@PtNi<sub>3</sub>-500 delivers an ultralow overpotential of 21 mV at 10 mA cm<sup>−2</sup> for HER under acidic conditions and a low onset potential of 1.27 V for UOR under alkaline conditions, surpassing monometallic Pt and Ni counterparts. When employed in an asymmetric acid-alkaline electrolyzer (HER/UOR), Pt@PtNi<sub>3</sub>-500 achieves a 68.3 % reduction in electrical energy consumption for H<sub>2</sub> production compared to traditional alkaline water splitting (HER/OER). Mechanistic investigations reveal that appropriate Ni incorporation in Pt@PtNi<sub>3</sub> increases the occupancy of Pt 5<em>d</em>–H 1<em>s</em> antibonding orbitals, which not only reinforces H<sup>+</sup> adsorption but also weakens the overly strong H∗ binding. Simultaneously, it reduces the energy barrier for ∗NH<sub>2</sub> dehydrogenation, thereby synergistically accelerating both H<sub>2</sub> generation and urea decomposition. This work provides new insights into the design of alloy electrocatalysts for high-efficiency H<sub>2</sub> production.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 12","pages":"Article 100159"},"PeriodicalIF":13.5,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144892887","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
Composition engineering in covalent organic frameworks for tailored photocatalysis 用于定制光催化的共价有机框架的组成工程
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-12-01 Epub Date: 2025-08-29 DOI: 10.1016/j.actphy.2025.100176
Yihong Shao , Rongchen Shen , Song Wang , Shijie Li , Peng Zhang , Xin Li
{"title":"Composition engineering in covalent organic frameworks for tailored photocatalysis","authors":"Yihong Shao ,&nbsp;Rongchen Shen ,&nbsp;Song Wang ,&nbsp;Shijie Li ,&nbsp;Peng Zhang ,&nbsp;Xin Li","doi":"10.1016/j.actphy.2025.100176","DOIUrl":"10.1016/j.actphy.2025.100176","url":null,"abstract":"<div><div>The harmful effects of the energy crisis and environmental degradation are becoming increasingly severe, which urgently demands the advancement of eco-friendly and sustainable production techniques. Direct conversion of abundant solar energy into chemical energy represents a promising green and efficient technological solution. In this process, photocatalysts play a pivotal role. Covalent organic frameworks (COFs), a class of porous materials interconnected by covalent bonds, exhibit exceptional potential for photocatalysis due to their high surface area, excellent crystallinity, and tunable structures. This review discusses the roles of compositional regulation in enhancing the photocatalytic performance of COFs, including modulating light absorption, increasing active sites, promoting exciton dissociation, and improving carrier separation. Furthermore, computational and mechanistic characterization methods are also discussed. More importantly, the key strategies in compositional regulation, such as heteroatom engineering, metal single-atom engineering, ion engineering, functional group engineering, Donor-Acceptor (D-A) molecular engineering, side chain engineering, multi-component engineering, isomerism engineering, conjugate bridge engineering, single-molecule junction engineering, and interlayer engineering, are carefully summarized. Moreover, their diversified modification strategies and applications in photocatalytic hydrogen (H<sub>2</sub>) evolution, hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production, and carbon dioxide (CO<sub>2</sub>) reduction are also addressed. Finally, the current challenges and future opportunities for COF-based photocatalysis are outlined.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 12","pages":"Article 100176"},"PeriodicalIF":13.5,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145118508","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
Inorganic-organic CdS/YBTPy S-scheme photocatalyst for efficient hydrogen production and its mechanism 无机-有机CdS/YBTPy s型高效产氢光催化剂及其机理
IF 13.5 2区 化学
物理化学学报 Pub Date : 2025-12-01 Epub Date: 2025-08-21 DOI: 10.1016/j.actphy.2025.100158
Mian Wei , Chang Cheng , Bowen He , Bei Cheng , Kezhen Qi , Chuanbiao Bie
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