IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102448

Scott Jensen , Brendan T. Sullivan , Daniel A. Hartzler , Irina Kosheleva , Robert W. Henning , Allison Page , Yulia Pushkar

{"title":"Challenges of observing O–O bond formation in the Mn4Ca cluster of photosystem II","authors":"Scott Jensen , Brendan T. Sullivan , Daniel A. Hartzler , Irina Kosheleva , Robert W. Henning , Allison Page , Yulia Pushkar","doi":"10.1016/j.chempr.2025.102448","DOIUrl":"10.1016/j.chempr.2025.102448","url":null,"abstract":"<div><div>Photosystem II (PS II) sustains the biosphere by enabling oxygen evolution in the S3-to-S0 transition (duration ∼1–2 ms) of its catalytic cycle. Using time-resolved Mn Kβ X-ray emission spectroscopy, we observed spectroscopic changes (which were unimpeded in D2O buffer) consistent with a modified electronic structure as early as ∼50 μs in the transition. These changes are consistent with the reduction of the Mn centers at the ∼50–200 μs time window in H2O and at ∼50–500 μs in D2O, ahead of the reduction of the redox-active TyrZ⋅+. These results indicate the multi-step nature of O–O bond formation and O2 release by the oxygen-evolving complex (OEC), where an O–O bond is most likely formed prior to the final electron-transfer step. The D2O-induced extension of up to ∼500 μs in the lifetime of the early transient state of a possible peroxo nature opens it up to further spectroscopic and structural analysis.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 7","pages":"Article 102448"},"PeriodicalIF":19.1,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144588885","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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-printing technologies for C1 chemistry C1化学的3d打印技术

IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102614

Jing Zhao , Xiaobo Peng , Lilong Jiang , Kang Cheng , Jincan Kang , Qinghong Zhang , Noritatsu Tsubaki , Ye Wang

引用次数: 0

Precision comonomer sequence enables selective thermodynamic degradation of vinyl copolymers 精密共聚物序列使乙烯基共聚物的选择性热力学降解

IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102648

Francesca D. Eckstrom , Eugene Y.-X. Chen

引用次数: 0

Transformable quadruply interpenetrated cage with multiple states of different reactivities 可变形的四层互穿笼，具有不同反应性的多种状态

IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102453

Tsukasa Abe , Yutong Zhang , Keisuke Takeuchi , Shuichi Hiraoka

{"title":"Transformable quadruply interpenetrated cage with multiple states of different reactivities","authors":"Tsukasa Abe , Yutong Zhang , Keisuke Takeuchi , Shuichi Hiraoka","doi":"10.1016/j.chempr.2025.102453","DOIUrl":"10.1016/j.chempr.2025.102453","url":null,"abstract":"<div><div>Molecular self-assemblies with multiple tunable pockets are potentially functional molecules that generate multiple states. Pd4L8 interpenetrated cages (ICs), in which two Pd2L4 cages are quadruply interpenetrated, have three correlating, tunable pockets for anions. Here, we report six ICs that bind halide ions (F− and Cl−), which we rationally designed on the basis of the anion matching index (AMI). They have different numbers and positions of F− and Cl− in their pockets. Three ICs are stable, and the other three are metastable. The outer anions in the stable ICs are selectively exchanged under kinetic control. The three thermodynamically stable ICs, whose suitability of anions was different only within 2 Å, showed totally different reactivities with BF3 and Ag+, and the IC with three Cl− was transformable into [2]-catenane by unusual ligand exchanges. A total of seven states were generated, affording a complicated network in response to halide ions, Lewis acids, Lewis bases, and Ag+.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 7","pages":"Article 102453"},"PeriodicalIF":19.1,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144588886","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

One-shot synthesis of BN-embedded hexabenzocoronene via a dearomative triple borylation 脱芳三硼化反应一次性合成bn包埋六苯并二苯甲醚

IF 23.5 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102655

Soichiro Nakatsuka, Takehiro Yamamoto, Hiroaki Abe, Shione Kiriyama, Masashi Mamada, Nobuhiro Yasuda, Susumu Oda, Chihaya Adachi, Takuji Hatakeyama

{"title":"One-shot synthesis of BN-embedded hexabenzocoronene via a dearomative triple borylation","authors":"Soichiro Nakatsuka, Takehiro Yamamoto, Hiroaki Abe, Shione Kiriyama, Masashi Mamada, Nobuhiro Yasuda, Susumu Oda, Chihaya Adachi, Takuji Hatakeyama","doi":"10.1016/j.chempr.2025.102655","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102655","url":null,"abstract":"The missing BN isostere of coronene, 2a1,6a1,10b1-triaza-2b,6b,10b-triborahexabenzo[a,d,g,j,m,p]coronene, was synthesized in a one-shot procedure from 2,4,6-tribenzhydryl-1,3,5-triazine via a dearomative triple borylation. In the crystalline state, the resulting nearly D3-symmetric molecule forms an efficient 3D π-stacking network, with disorder observed in the B–N and C=C bonds. Density functional theory (DFT) calculations of electronic couplings predict a promising potential for applications in organic semiconducting materials. The introduction of six additional methyl groups suppressed this disorder, enabling precise bond-length alternation analysis. Notably, the incorporation of three BN units into the spoke positions of the coronene core induced a paratropic ring current in the N3C3 central ring, a hypsochromic shift in absorption and emission maxima, and an enhanced photoluminescence quantum yield. Furthermore, selective single and double borylations of 2,4,6-tribenzhydryl-1,3,5-triazine were demonstrated, alongside a dearomative triple borylation of its benzothiophene analog. These findings may accelerate advances in both fundamental and applied chemistry based on BN/CC isosterism.","PeriodicalId":268,"journal":{"name":"Chem","volume":"21 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144594875","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Enzymatic DNA orthogonal chemistry for multi-cancer diagnosis 酶DNA正交化学用于多种肿瘤诊断

IF 23.5 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102656

Dongsheng Mao, Hongquan Gou, Wen Chen, Rui Zhu, Fanping Zhang, Wentao Zhang, Yuanyuan Zhang, Xiaozhi Huang, Min Li, Wenxing Li, Bing Shen, Xiaoli Zhu

{"title":"Enzymatic DNA orthogonal chemistry for multi-cancer diagnosis","authors":"Dongsheng Mao, Hongquan Gou, Wen Chen, Rui Zhu, Fanping Zhang, Wentao Zhang, Yuanyuan Zhang, Xiaozhi Huang, Min Li, Wenxing Li, Bing Shen, Xiaoli Zhu","doi":"10.1016/j.chempr.2025.102656","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102656","url":null,"abstract":"Orthogonal detection of multiple targets is essential for precision medicine, but achieving this in homogeneous systems is challenging owing to coordination issues regarding reagents and detection platforms. Here, we developed an enzymatic DNA orthogonal chemistry-based 3D spectral fingerprint (EzDo-CRAFT) platform, which integrates nicking endonuclease-based orthogonality with excitation-emission matrix (EEM) spectroscopy-based 3D signal resolution. Notably, we discovered that the nicking endonuclease Nt.BstNBI exhibits sensitivity to variable recognition sites and that their reaction processes are highly orthogonal, which laid the foundation for EzDo-CRAFT. Moreover, EEM spectroscopy effectively overcomes the limitations of spectral overlap and provides 3D spectral fingerprint features with high information density. The EzDo-CRAFT platform enabled one-pot detection of 10 targets across bladder cancer, prostate cancer, kidney cancer, and healthy individuals, using clinical urine samples, demonstrating high sensitivity (82.7%, 95% CI: 63.5%–93.5%) and specificity (81.8%, 95% CI: 47.8%–96.8%). This EzDo-CRAFT platform demonstrates an innovative application of nicking endonucleases and their potential for advancing precision medicine.","PeriodicalId":268,"journal":{"name":"Chem","volume":"47 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144594876","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Challenges and perspectives for the perovskite module research 过氧化物模块研究的挑战和前景

IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102542

Runda Li , Libing Yao , Jingyi Sun , Zengyi Sun , Kai Zhang , Jingjing Xue , Rui Wang

{"title":"Challenges and perspectives for the perovskite module research","authors":"Runda Li , Libing Yao , Jingyi Sun , Zengyi Sun , Kai Zhang , Jingjing Xue , Rui Wang","doi":"10.1016/j.chempr.2025.102542","DOIUrl":"10.1016/j.chempr.2025.102542","url":null,"abstract":"<div><div>With rapid technological advancements, perovskite photovoltaics are approaching the final stage of commercialization. However, challenges arise due to differences between the fabrication processes for large-scale perovskite solar modules (PSMs) and laboratory-scale perovskite solar cells (PSCs). In this perspective, we highlight key obstacles in the transition from PSCs to PSMs across three main fabrication stages: precursor solution preparation, large-scale perovskite deposition, and post-treatment procedures for modules. Beyond addressing long-term stability, we emphasize critical yet often overlooked factors: reproducibility, cost, quality control, and sustainability in PSM manufacture. Finally, we provide our outlook by posing three controversial questions: which type of PSMs will be finally commercialized, how to balance the device area and lateral resistance, and how to realize a stable supply of raw materials. We hope that this effort may provide insights into targeted scientific strategies that can bridge these gaps and facilitate the commercialization of perovskite photovoltaics.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 7","pages":"Article 102542"},"PeriodicalIF":19.1,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837101","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Photocatalytic product-selective reduction of CO2, CO, and carbonates 光催化产物选择性还原CO2， CO和碳酸盐

IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102450

Rohan Bhimpuria , Monika Tomar , Anders Thapper , Mårten Ahlquist , K. Eszter Borbas

引用次数: 0

Encapsulation of metal nanoclusters into hydrogen-bonded organic frameworks for double-response-reverse ammonia fluorescence sensing 金属纳米团簇包封成氢键有机框架用于双响应-反向氨荧光传感

IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102457

Yuxin Wang , Jia Yao , Shitao Wu , Chao Zhi , Lifei Yin , Zhengxuan Song , Jing Wang , Lixia Ling , Yanhang Ma , Daliang Zhang , Jinping Li , Libo Li , Banglin Chen

{"title":"Encapsulation of metal nanoclusters into hydrogen-bonded organic frameworks for double-response-reverse ammonia fluorescence sensing","authors":"Yuxin Wang , Jia Yao , Shitao Wu , Chao Zhi , Lifei Yin , Zhengxuan Song , Jing Wang , Lixia Ling , Yanhang Ma , Daliang Zhang , Jinping Li , Libo Li , Banglin Chen","doi":"10.1016/j.chempr.2025.102457","DOIUrl":"10.1016/j.chempr.2025.102457","url":null,"abstract":"<div><div>Ammonia (NH3) is considered a biomarker of liver and kidney diseases; sensitive and visible fluorescence sensors are expected to achieve quantitative detection of breath NH3, although low accuracy makes them difficult to apply in breath tests. Herein, we adopted a “double-response-reverse fluorescence” strategy via in situ encapsulation of a metal nanocluster (MNC) into a hydrogen-bonded organic framework, successfully constructing an ultra-accurate ratiometric fluorescence sensor (Pt2Cu4@HOF-101). With a combination of π-conjugated HOF and luminescent MNC, two kinds of NH3 recognition sites were preciously assembled and raised significant orbital energy changes, thus realizing a strong response to trace NH3. The precision-assembled Pt2Cu4@HOF-101 has been eloquently inspected by three-dimensional electron diffraction, which comprehensively uncovered the structure-induced double-response-reverse sensing mechanism. Notably, Pt2Cu4@HOF-101 enabled exact quantification of the NH3 exhaled, and the measured expiratory concentration was highly positively correlated with the blood test, which offers a new approach for the painless diagnosis of liver and kidney diseases.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 7","pages":"Article 102457"},"PeriodicalIF":19.1,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539184","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Practical flow battery diagnostics enabled by chemically mediated monitoring 通过化学介导监测实现实用的液流电池诊断技术

IF 19.1 1区化学

Chem Pub Date : 2025-07-10 DOI: 10.1016/j.chempr.2025.102543

Mark E. Carrington , Loh Min Yi , Erlendur Jónsson , Clare P. Grey

引用次数: 0

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