JACS Au

Cun Liu

Botao Qiao

Tao Zhang

Integration of Single Atoms for Tandem Catalysis

单原子集成用于串联催化

Coenzyme F430, the prosthetic group of methyl coenzyme M reductase (MCR), is a key compound in methane metabolism. We applied coenzyme F430 as a function-specific biomarker of methanogenesis to subsurface marine sediments collected below the sulfate reduction zone to investigate the distribution and activity of methanogens. In addition, we examined the kinetics of the epimerization of coenzyme F430, which is the first stage of the degradation process after cell death, at various temperatures (4, 15, 34, 60 °C) and pH (5, 7, 9) conditions, which cover in situ conditions of drilled sediments used in this study. The degradation experiments revealed that the kinetics of the epimerization well follow the thermodynamic laws, and the half-life of coenzyme F430 is decreasing from 304 days to 11 h with increasing the in situ temperature. It indicates that the native F430 detected in the sediments is derived from living methanogens, because the abiotic degradation of F430 is much faster than the sedimentation rate and will not be fossilized. Based on coenzyme F430 analysis and degradation experiments, the native form of F430 detected in subseafloor sediments off the Shimokita Peninsula originates from living methanogen cells, which is protected from degradation in cells but disappears soon after cell death. The biomass of methanogens calculated from in situ F430 concentration and F430 contents in cultivable methanogen species decreases by 2 orders of magnitude up to a sediment depth of 2.5 km, with a maximum value at ∼70 m below the seafloor (mbsf), while the proportion of methanogens to the total prokaryotic cell abundance increases with the depth, which is 1 to 2 orders of magnitude higher than expected previously. Our results indicate the presence of undetectable methanogens using conventional techniques.

Masanori Kaneko

Yoshinori Takano

Masashi Kamo

Kazuya Morimoto

Takuro Nunoura

Naohiko Ohkouchi

Insights into the Methanogenic Population and Potential in Subsurface Marine Sediments Based on Coenzyme F430 as a Function-Specific Biomarker

基于功能特异性生物标志物辅酶F430的地下海洋沉积物中产甲烷种群及潜力研究

In the past decade, isolated single atoms have been successfully dispersed on various substrates, with their potential applications being intensively investigated in different reactions. While the essential target of research in single-atom catalysis is the precise synthesis of stable single-atom catalysts (SACs) with clear configurations and impressive catalytic performance, theoretical investigations have also played important roles in identifying active sites, revealing catalytic mechanisms, and establishing structure–activity relationships. Nevertheless, special attention should still be paid in theoretical works to the particularity of SACs. In this Perspective, we will summarize the theoretical progress made on the understanding of the rich phenomena in single-atom catalysis. We focus on the determination of local structures of SACs via comparison between experiments and simulations, the discovery of distinctive catalytic mechanisms induced by multiadsorption, synergetic effects, and dynamic evolutions, to name a few, the proposal of criteria for theoretically designing SACs, and the extension of original concepts of single-atom catalysis. We hope that this Perspective will inspire more in-depth thinking on future theoretical studies of SACs.

Wenhua Zhang

Qiang Fu

Qiquan Luo

Li Sheng

Jinlong Yang

Understanding Single-Atom Catalysis in View of Theory

The accurate and timely detection of disease biomarkers at the point-of-care is essential to ensuring effective treatment and epidemiological surveillance. Here, we report the selection and engineering of RNA-cleaving DNAzymes that respond to specific genetic markers and amplify detection signals. Because the target-specific activation of gene-specific DNAzymes (gDz) is like the trans-cleavage activity of clustered regularly interspaced short palindromic repeats (CRISPR) CRISPR-associated (Cas) machinery, we further developed a CRISPR-like assay using RNA-cleaving DNAzyme coupled with isothermal sequence and signal amplification (CLARISSA) for nucleic acid detection in clinical samples. Building on the high sequence specificity and orthogonality of gDzs, CLARISSA is highly versatile and expandable for multiplex testing. Upon integration with an isothermal recombinase polymerase amplification, CLARISSA enabled the detection of human papillomavirus (HPV) 16 in 189 cervical samples collected from cervical cancer screening participants (n = 189) with 100% sensitivity and 97.4% specificity, respectively. A multiplexed CLARISSA further allowed the simultaneous analyses of HPV16 and HPV18 in 46 cervical samples, which returned clinical sensitivity of 96.3% for HPV16 and 83.3% for HPV18, respectively. No false positives were found throughout our tests. Besides the fluorescence readout using fluorogenic reporter probes, CLARISSA is also demonstrated to be fully compatible with a visual lateral flow readout. Because of the high sensitivity, accessibility, and multiplexity, we believe CLARISSA is an ideal CRISPR-Dx alternative for clinical diagnosis in field-based and point-of-care applications.

Lu Gao

Ke Yi

Yun Tan

Chen Guo

Danxi Zheng

Chenlan Shen

Feng Li

Engineering Gene-Specific DNAzymes for Accessible and Multiplexed Nucleic Acid Testing

Biocatalysis is an effective approach for producing chiral drug intermediates that are often difficult to synthesize using traditional chemical methods. A time-efficient strategy is required to accelerate the directed evolution process to achieve the desired enzyme function. In this research, we evaluated machine learning-assisted directed evolution as a potential approach for enzyme engineering, using a moderately diastereoselective ketoreductase library as a model system. Machine learning-assisted directed evolution and traditional directed evolution methods were compared for reducing (±)-tetrabenazine to dihydrotetrabenazine via kinetic resolution facilitated by BsSDR10, a short-chain dehydrogenase/reductase from

Chenming Huang

Li Zhang

Tong Tang

Haijiao Wang

Yingqian Jiang

Hanwen Ren

Yitian Zhang

Jiali Fang

Wenhe Zhang

Xian Jia

Song You

Bin Qin

Application of Directed Evolution and Machine Learning to Enhance the Diastereoselectivity of Ketoreductase for Dihydrotetrabenazine Synthesis

Maninderjeet Singh

Saurabh Kr. Tiwary

Roushanak Nejat

Jack F. Douglas

Alamgir Karim

Anomalously High Dielectric Strength and Capacitive Energy Density of Thin Entangled Glassy Polymer Films

异常高的介电强度和薄缠结玻璃态聚合物薄膜的电容性能量密度

Leyla R. Valerio

Sabyasachi Roy Chowdhury

Rob Lewis

Kathryn E. Knowles

Bess Vlaisavljevich

Ellen M. Matson

Photoluminescence of a Uranium(IV) Alkoxide Complex

铀(IV)醇盐配合物的光致发光

Ya Cao

Jianan Xia

Lijuan Li

Yujing Zeng

Jing Zhao

Genxi Li

Electrochemical Biosensors for Cancer Diagnosis: Multitarget Analysis to Present Molecular Characteristics of Tumor Heterogeneity

用于癌症诊断的电化学生物传感器：多靶点分析以呈现肿瘤异质性的分子特征

Tong Zhang

Arindam Ghosh

Lisa Behringer-Pließ

Lata Chouhan

Ana V. Cunha

Remco W. A. Havenith

Eugenia Butkevich

Lei Zhang

Olalla Vázquez

Elke Debroye

Jörg Enderlein

Shoubhik Das

Proton Tunneling Allows a Proton-Coupled Electron Transfer Process in the Cancer Cell

质子隧穿使癌细胞中的质子耦合电子转移过程成为可能

Akash Warty

Amy Chen

Dat T. Tran

Harrison Kraus

Taylor J. Woehl

Dongxia Liu

Electrochemical Synthesis of Zeolite Coatings with Controlled Crystal Polymorphism and Self-Regulating Growth

电化学合成具有受控晶体多型性和自调节生长的沸石涂层

短名	JACS. Au.
Journal Impact	8.30
国际分区	CHEMISTRY, MULTIDISCIPLINARY(Q1)

ISSN	2691-3704
h-index	36

涉及主题	化学有机化学物理生物生物化学材料科学量子力学工程类催化作用物理化学遗传学纳米技术核磁共振计算机科学化学工程复合材料冶金医学
出版信息	出版商: American Chemical Society，出版周期: ，期刊类型: journal，开源期刊: 是
基本数据	创刊年份: 2021，原创研究文献占比: 99.61%，自引率:2.40%， Gold OA占比: 71.67%
期刊费用	$3500详情
平均审稿周期	网友分享经验：10 Weeks

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