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Dramatic switchable polarities in conduction type and self-driven photocurrent of BiI3 via pressure engineering. 通过压力工程实现BiI3导电型和自驱动光电流的显著极性转换。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-12-03 eCollection Date: 2025-01-01 DOI: 10.1093/nsr/nwae419
Lei Yue, Fuyu Tian, Ran Liu, Zonglun Li, Ruixin Li, Chenyi Li, Yanchun Li, Dongliang Yang, Xiaodong Li, Quanjun Li, Lijun Zhang, Bingbing Liu

The intentional manipulation of carrier characteristics serves as a fundamental principle underlying various energy-related and optoelectronic semiconductor technologies. However, achieving switchable and reversible control of the polarity within a single material to design optimized devices remains a significant challenge. Herein, we successfully achieved dramatic reversible p-n switching during the semiconductor‒semiconductor phase transition in BiI3 via pressure, accompanied by a substantial improvement in their photoelectric properties. Carrier polarity flipping was monitored by measuring the photocurrent dominated by the photothermoelectric (PTE) effect in a zero-bias two-terminal device. Accompanying the p-n transition, a switch between positive and negative photocurrents was observed in BiI3, providing a feasible method to determine the conduction type of materials via photoelectric measurements. Furthermore, the combined effects of the photoconductivity and PTE mechanism improved the photoresponse and extended the detection bandwidth to encompass the optical communication waveband (1650 nm) under an external bias. The remarkable photoelectric properties were attributed to the enhanced energy band dispersion and increased charge density of BiI3 under pressure. These findings highlight the effective and flexible modulation of carrier properties through pressure engineering and provide a foundation for designing and implementing multifunctional logic circuits and optoelectronic devices.

有意操纵载流子特性是各种能源相关和光电子半导体技术的基本原理。然而,在单一材料中实现可切换和可逆的极性控制以设计优化器件仍然是一个重大挑战。在此,我们成功地在BiI3的半导体-半导体相变过程中通过压力实现了戏剧性的可逆p-n开关,并伴随着光电性能的实质性改善。通过测量零偏压双端器件中以光热电(PTE)效应为主的光电流来监测载流子极性翻转。随着p-n跃迁,在BiI3中观察到正负光电流之间的切换,为通过光电测量确定材料的导电类型提供了一种可行的方法。此外,光电导率和PTE机制的联合作用改善了光响应,并将检测带宽扩展到包含外部偏压下的光通信波段(1650 nm)。BiI3在压力下的能带色散增强和电荷密度增加是其显著的光电性能的主要原因。这些发现强调了通过压力工程有效和灵活地调制载流子特性,并为设计和实现多功能逻辑电路和光电子器件提供了基础。
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引用次数: 0
The roadmap of two-dimensional materials toward next-generation image sensor. 二维材料迈向下一代图像传感器的路线图。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-30 eCollection Date: 2024-12-01 DOI: 10.1093/nsr/nwae431
Na Zhang, Decai Ouyang, Yuan Li, Tianyou Zhai

This Prospective highlights the advances and challenges of 2D materials regarding the materials preparation, device integration, multifunctional applications, and comments on their potential as transformative candidates for future image sensors.

本展望强调了二维材料在材料制备、器件集成、多功能应用方面的进步和挑战,并评论了它们作为未来图像传感器变革候选者的潜力。
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引用次数: 0
Artificial intelligence and biological research. 人工智能和生物研究。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-28 eCollection Date: 2024-11-01 DOI: 10.1093/nsr/nwae415
Chung-I Wu, Cai Li
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引用次数: 0
High-performance MXene films by sequential bridging. 顺序桥接的高性能MXene薄膜。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-28 eCollection Date: 2024-12-01 DOI: 10.1093/nsr/nwae432
Xianhu Liu, Jingna Zhang, Chuntai Liu, Changyu Shen
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引用次数: 0
Two-dimensional Health State Map to define metabolic health using separated static and dynamic homeostasis features: a proof-of-concept study. 使用分离的静态和动态稳态特征定义代谢健康的二维健康状态图:概念验证研究。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-26 eCollection Date: 2025-01-01 DOI: 10.1093/nsr/nwae425
Yanpu Wu, Xinyan Zhang, Liang Sun, Qingqing Wu, Xiaoping Liu, Yueyi Deng, Zhenzhen Lu, Zhongxia Li, Chaoming Deng, Ruikun He, Luyun Zhang, Rong Zeng, Xuguang Zhang, Luonan Chen, Xu Lin

Defining metabolic health is critical for the earlier reversing of metabolic dysfunction and disease, and fasting-based diagnosis may not adequately assess an individual's metabolic adaptivity under stress. We constructed a novel Health State Map (HSM) comprising a Health Phenotype Score (HPS) with fasting features alone and a Homeostatic Resilience Score (HRS) with five time-point features only (t = 30, 60, 90, 180, 240 min) following a standardized mixed macronutrient tolerance test (MMTT). Among 111 Chinese adults, when the same set of fasting and post-MMTT data as for the HSM was used, the mixed-score was highly correlated with the HPS. The HRS was significantly associated with metabolic syndrome prevalence, independently of the HPS (OR [95% CI]: 0.41 [0.18, 0.92]) and the mixed-score (0.34 [0.15, 0.69]). Moreover, the HRS could discriminate metabolic characteristics unseparated by the HPS and the mixed-score. Participants with higher HRSs had better metabolic traits than those with lower HRSs. Large interpersonal variations were also evidenced by evaluating postprandial homeostatic resiliencies for glucose, lipids and amino acids when participants had similar overall HRSs. Additionally, the HRS was positively associated with physical activity level and specific gut microbiome structure. Collectively, our HSM model might offer a novel approach to precisely define an individual's metabolic health and nutritional capacity.

定义代谢健康对于代谢功能障碍和疾病的早期逆转至关重要,基于禁食的诊断可能无法充分评估个体在压力下的代谢适应性。我们构建了一个新的健康状态图(HSM),包括单独具有禁食特征的健康表型评分(HPS)和仅具有五个时间点特征(t = 30,60,90,180,240分钟)的稳态恢复评分(HRS),然后进行标准化的混合宏量营养素耐受性试验(MMTT)。在111名中国成年人中,当使用与HSM相同的禁食和mmtt后数据时,混合评分与HPS高度相关。HRS与代谢综合征患病率显著相关,独立于HPS (OR [95% CI]: 0.41[0.18, 0.92])和混合评分(0.34[0.15,0.69])。此外,HRS还可以区分HPS和混合评分未分离的代谢特征。高HRSs的参与者比低HRSs的参与者有更好的代谢特征。当参与者的总体HRSs相似时,通过评估餐后葡萄糖、脂质和氨基酸的体内平衡弹性,也证明了人与人之间的巨大差异。此外,HRS与身体活动水平和特定肠道微生物群结构呈正相关。总的来说,我们的HSM模型可能提供一种精确定义个体代谢健康和营养能力的新方法。
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引用次数: 0
Unraveling climate change-induced compound low-solar-low-wind extremes in China. 解开中国气候变化引起的复合低太阳-低风极端现象。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-25 eCollection Date: 2025-01-01 DOI: 10.1093/nsr/nwae424
Licheng Wang, Yawen Liu, Lei Zhao, Xi Lu, Liangdian Huang, Yana Jin, Steven J Davis, Amir Aghakouchak, Xin Huang, Tong Zhu, Yue Qin

China's pursuit of carbon neutrality targets hinges on a profound shift towards low-carbon energy, primarily reliant on intermittent and variable, yet crucial, solar and wind power sources. In particular, low-solar-low-wind (LSLW) compound extremes present a critical yet largely ignored threat to the reliability of renewable electricity generation. While existing studies have largely evaluated the impacts of average climate-induced changes in renewable energy resources, comprehensive analyses of the compound extremes and, particularly, the underpinning dynamic mechanisms remain scarce. Here we show the dynamic evolution of compound LSLW extremes and their underlying mechanisms across China via coupling multi-model simulations with diagnostic analysis. Our results unveil a strong topographic dependence in the frequency of compound LSLW extremes, with a national average frequency of 16.4 (10th-90th percentile interval ranges from 5.3 to 32.6) days/yr, when renewable energy resources in eastern China are particularly compromised (∼80% lower than that under an average climate). We reveal a striking increase in the frequency of LSLW extremes, ranging from 12.4% under SSP126 to 60.2% under SSP370, primarily driven by both renewable energy resource declines and increasingly heavily-tailed distributions, resulting from weakened meridional temperature (pressure) gradient, increased frequency of extremely dense cloud cover and additional distinctive influence of increased aerosols under SSP370. Our study underscores the urgency of preparing for significantly heightened occurrences of LSLW events in a warmer future, emphasizing that such climate-induced compound LSLW extreme changes are not simply by chance, but rather projectable, thereby underscoring the need for proactive adaptation strategies. Such insights are crucial for countries navigating a similar transition towards renewable energy.

中国对碳中和目标的追求取决于向低碳能源的深刻转变,主要依赖间歇性、可变但至关重要的太阳能和风能。特别是,低太阳能低风能(LSLW)复合极端情况对可再生能源发电的可靠性构成了一个严重但在很大程度上被忽视的威胁。虽然现有的研究在很大程度上评估了气候引起的平均变化对可再生能源的影响,但对复合极端情况的综合分析,特别是对基本动态机制的分析仍然很少。本文通过多模式模拟与诊断分析相结合的方法,揭示了中国地区复合极端低潮的动态演变及其潜在机制。我们的研究结果揭示了复合LSLW极端事件的频率具有很强的地形依赖性,全国平均频率为16.4天/年(第10 -90百分位数间隔为5.3至32.6),当中国东部的可再生能源资源受到特别损害时(比平均气候下低约80%)。我们发现,极端LSLW的频率显著增加,从SSP126下的12.4%增加到SSP370下的60.2%,这主要是由可再生能源资源减少和经向温度(压力)梯度减弱、极密云覆盖频率增加以及SSP370下气溶胶增加的额外显著影响导致的重尾分布的增加所驱动的。我们的研究强调了在一个更温暖的未来,为LSLW事件显著增加的发生做好准备的紧迫性,强调了这种由气候引起的复合LSLW极端变化不仅仅是偶然的,而是可以预测的,因此强调了主动适应策略的必要性。这些洞见对于正在进行类似的向可再生能源转型的国家至关重要。
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引用次数: 0
Controlled van der Waals epitaxy of 2D single-crystal molecular film. 二维单晶分子膜的可控范德华外延。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-25 eCollection Date: 2024-12-01 DOI: 10.1093/nsr/nwae405
Xinghui Liu, Young Hee Lee
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引用次数: 0
Unlocking new possibilities in ionic thermoelectric materials: a machine learning perspective. 打开离子热电材料的新可能性:机器学习的视角。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-23 eCollection Date: 2025-01-01 DOI: 10.1093/nsr/nwae411
Yidan Wu, Dongxing Song, Meng An, Cheng Chi, Chunyu Zhao, Bing Yao, Weigang Ma, Xing Zhang

The high thermopower of ionic thermoelectric (i-TE) materials holds promise for miniaturized waste-heat recovery devices and thermal sensors. However, progress is hampered by laborious trial-and-error experimentations, which lack theoretical underpinning. Herein, by introducing the simplified molecular-input line-entry system, we have addressed the challenge posed by the inconsistency of i-TE material types, and present a machine learning model that evaluates the Seebeck coefficient with an R 2 of 0.98 on the test dataset. Using this tool, we experimentally identify a waterborne polyurethane/potassium iodide ionogel with a Seebeck coefficient of 41.39 mV/K. Furthermore, interpretable analysis reveals that the number of rotatable bonds and the octanol-water partition coefficient of ions negatively affect Seebeck coefficients, which is corroborated by molecular dynamics simulations. This machine learning-assisted framework represents a pioneering effort in the i-TE field, offering significant promise for accelerating the discovery and development of high-performance i-TE materials.

离子热电(i-TE)材料的高热功率为小型化废热回收装置和热传感器带来了希望。然而,缺乏理论基础的艰苦的试错实验阻碍了进展。在此,通过引入简化的分子输入线输入系统,我们解决了i-TE材料类型不一致带来的挑战,并提出了一个机器学习模型,该模型在测试数据集上评估塞贝克系数的r2为0.98。利用该工具,我们实验鉴定了一种塞贝克系数为41.39 mV/K的水性聚氨酯/碘化钾离子凝胶。此外,可解释分析表明,可旋转键数和离子的辛醇-水分配系数对塞贝克系数有负影响,这一点得到了分子动力学模拟的证实。这种机器学习辅助框架代表了i-TE领域的开创性努力,为加速高性能i-TE材料的发现和开发提供了重大希望。
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引用次数: 0
Molecular modification enables CO2 electroreduction to methane on platinum surface in acidic media. 分子修饰使CO2在酸性介质中电还原为铂表面的甲烷。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-19 eCollection Date: 2024-12-01 DOI: 10.1093/nsr/nwae361
Hengpan Yang, Huizhu Cai, Deliang Li, Yan Kong, Shangzhao Feng, Xingxing Jiang, Qi Hu, Chuanxin He

Cu-based materials can produce hydrocarbons in CO2 electroreduction (CO2RR), but their stability still needs to be enhanced particularly in acidic media. Metallic Pt is highly stable in both acidic and alkaline media, yet rarely utilized in CO2RR, due to the competitive activity in hydrogen evolution reaction (HER). In this research, abundant thionine (Th) molecules are stably confined within Pt nanocrystals via a molecular doping strategy. The Pt surface is successfully modulated by these Th molecules, and thereby the dominant HER activity is converted to CO2RR activity. CO2 could be electroreduced to CH4 using organic molecule-modified Pt-based catalysts for the first time. Specifically, this composite catalyst maintains more than 100-hour stability in strong acid conditions (pH 1), even comparable to those state-of-the-art CO2RR catalysts. In-situ spectroscopic analysis and theoretical calculations reveal that the molecular modification can decrease the energy barrier for *COOH formation, and guarantee the sufficient local *H near Pt surface. Additionally, the *H derived from H2O dissociation is favorable for the *CO hydrogenation pathway towards *CHO, eventually leading to the formation of CH4. This strategy might be easily applied to microenvironment and interface regulation in other electrocatalytic reactions.

铜基材料在CO2电还原(CO2RR)中可以产生碳氢化合物,但其稳定性仍有待提高,特别是在酸性介质中。金属Pt在酸性和碱性介质中都具有很高的稳定性,但由于析氢反应(HER)中的竞争活性,在CO2RR中很少被利用。在本研究中,通过分子掺杂策略,将丰富的硫氨酸(Th)分子稳定地限制在Pt纳米晶体中。这些Th分子成功地调节了Pt表面,从而使主导的HER活性转化为CO2RR活性。首次使用有机分子修饰的pt基催化剂将CO2电还原为CH4。具体来说,这种复合催化剂在强酸条件下(pH值为1)保持超过100小时的稳定性,甚至可以与最先进的CO2RR催化剂相媲美。原位光谱分析和理论计算表明,分子修饰可以降低*COOH形成的能垒,保证Pt表面附近有足够的局部*H。另外,H2O解离生成的*H有利于*CO加氢生成*CHO,最终生成CH4。该策略可以很容易地应用于其他电催化反应的微环境和界面调节。
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引用次数: 0
Mercury records from natural archives reveal ecosystem responses to changing atmospheric deposition. 来自自然档案的汞记录揭示了生态系统对大气沉积变化的响应。
IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Pub Date : 2024-11-19 eCollection Date: 2024-12-01 DOI: 10.1093/nsr/nwae417
Qinqin Chen, Qingru Wu, Yuying Cui, Shuxiao Wang

Global ecosystems face mercury contamination, yet long-term data are scarce, hindering understanding of ecosystem responses to atmospheric Hg input changes. To bridge the data gap and assess ecosystem responses, we compiled and compared a mercury accumulation database from peat, lake, ice and marine deposits worldwide with atmospheric mercury deposition modelled by GEOS-Chem, focusing on trends, magnitudes, spatial-temporal distributions and impact factors. The mercury fluxes in all four deposits showed a 5- to 9-fold increase over 1700-2012, with lake and peat mercury fluxes that generally mirrored atmospheric deposition trends. Significant decreases in lake and peat mercury fluxes post-1950 in Europe evidenced effective environmental policies, whereas rises in East Asia, Africa and Oceania highlighted coal-use impacts, inter alia. Conversely, mercury fluxes in marine and high-altitude ecosystems did not align well with atmospheric deposition, emphasizing natural influences over anthropogenic impacts. Our study underscores the importance of these key regions and ecosystems for future mercury management.

全球生态系统面临汞污染,但长期数据缺乏,阻碍了对生态系统对大气汞输入变化的响应的理解。为了弥补数据差距并评估生态系统的响应,我们编译并比较了全球泥炭、湖泊、冰和海洋沉积物的汞积累数据库与GEOS-Chem模拟的大气汞沉积,重点关注趋势、幅度、时空分布和影响因素。在1700年至2012年期间,所有四个沉积物中的汞通量增加了5至9倍,湖泊和泥炭的汞通量大体上反映了大气沉积趋势。1950年后,欧洲湖泊和泥炭汞通量的显著减少证明了有效的环境政策,而东亚、非洲和大洋洲汞通量的增加则突出了煤炭使用的影响等。相反,海洋和高海拔生态系统中的汞通量与大气沉降不太一致,强调自然影响大于人为影响。我们的研究强调了这些关键区域和生态系统对未来汞管理的重要性。
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引用次数: 0
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