Journal of the American Chemical Society
·
2026
·
IF 16.6
Li Shuying,Wang Zhuo,Cao Yiqun,Ma Wei,Li Hao,Chen Tianzeng,Wang Yonghong,Zhang Peng,Liu Pengfei,Chu Biwu,Liu Chang,Liu Yongchun,Mu Yujing,Zhang Xiuhui,Wang Tao,Ma Qingxin,Francisco Joseph S.,He Hong
Reactive
chlorine species significantly influence atmospheric
chemistry,
yet their sources remain inadequately defined. We have discovered
a spontaneous formation pathway for substantial molecular chlorine
(Cl 2 ) from the oxidation of chloride (Cl – ) through interfacial oxidation by O 2 on acidic microdroplets.
This efficient interfacial reaction is facilitated by protons (H + ), which enrich Cl – at the gas–liquid
interface and mediate the electron-transfer process, concurrently
releasing gaseous Cl 2 and hydroxyl radicals (OH). Given
the prevalence of acidic, chloride-containing droplets in marine and
polluted urban environments, this formation mechanism constitutes
a substantial and previously unaccounted tropospheric chlorine source.
Unlike established mechanisms, this pathway generates active halogens
without consuming gaseous oxidants like O 3 or OH, instead
producing particulate reactive oxygen species (ROS). Consequently,
current atmospheric models likely underestimate the contribution of
reactive halogens to atmospheric oxidation capacity.
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2024
·
IF 14.4
Baoxin Ni,Peng Shen,Guiru Zhang,Jiajun Zhao,Honghe Ding,Yifan Ye,Zhouying Yue,Hui Yang,Hao Wei,Kun Jiang
Pt is a well-known benchmark catalyst in the acidic oxygen reduction reaction (ORR) that drives electrochemical O2-to-H2O conversion with maximum chemical energy-to-electricity efficiency. Once dispersing bulk Pt into isolated single atoms, however, the preferential ORR pathway remains a long-standing controversy due to their complex local coordination environment and diverse site density over substrates. Herein, using a set of carbon nanotube supported Pt–N–C single-atom catalysts, we demonstrate how the neighboring N dopants regulate the electronic structure of the Pt central atom and thus steer the ORR selectivity; that is, the O2-to-H2O2 conversion selectivity can be tailored from 10% to 85% at 0.3 V versus reversible hydrogen electrode. Moreover, via a comprehensive X-ray-radiated spectroscopy and shell-isolated nanoparticle-enhanced Raman spectroscopy analysis coupled with theoretical modeling, we reveal that a dominant pyridinic- and pyrrolic-N coordination within the first shell of Pt–N–C motifs favors the 4e– ORR, whereas the introduction of a second-shell graphitic-N dopant weakens *OOH binding on neighboring Pt sites and gives rise to a dominant 2e– ORR. These findings underscore the importance of the chemical environment effect for steering the electrochemical performance of single-atom catalysts.
研究领域:
电化学
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Juanjuan Jin,Changjun Yang,Bingguang Zhang,Kejian Deng
A highly efficient oxidation of amines including primary and secondary amines into imines using O 2 as the oxidant was realized by cobalt tetra(2-hydroxymethyl-1,4-dithiin)porphyrazine (CoPz(hmdtn) 4 ) under irradiation of visible light ( λ ≥ 420 nm). Particularly, the photocatalytic selective oxidation of benzylamine into N -benzylidenebenzylamine was thoroughly studied in order to get more insight into the reaction kinetics and mechanism for the oxidation of amine. The photocatalytic oxidation of benzylamine was observed to follow pseudo-first-order reaction kinetics. Moreover, a reasonable linear relationship between the log( k X / k H ) values and the Brown-Okamoto constant ( σ + ) parameters was obtained for oxidation of para - and meta -substituted benzylamines. Besides imine, the presence of other intermediate products such as NH-imine and H 2 O 2 was further evidenced in this photocatalytic system. Additionally, the reactive oxygen species (ROSs) generated in this photocatalytic process were confirmed by electron spin resonance (ESR) technique. The possible photocatalytic transformation pathway of amine into imine was also proposed, involving the dehydrogenation of amine to form NH-imine and the nucleophilic addition of NH-imine by free amine to afford the final imine.
研究领域:
化学
·
催化
·
光化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2015
·
IF 6.217
Chuan-tao Song,Bo-wen Huang,Xiao-zhen Liao,Xiao-min Liu,Hui Yang,Zi-feng Ma
Li–O 2 cell is considered as an ideal choice for the electric vehicles due to its high energy density , but is now suffering from the large charge polarization and low practical capacity. In this context, three-dimensional network macro-porous CoO synthesized via a sol–gel method is applied as an efficient catalyst in Li–O 2 cells to alleviate this situation. Compared to KB (Ketjen black EC600JD) based cells, the CoO/KB based cell exhibits much improved electrochemical performance at various current densities, including flatter discharge/charge plateau, lower polarization and higher specific capacity. In addition, the CoO/KB based cell maintains the discharge capacity up to 4500 mAh g −1 CoO/KB after being cycled at 0.1 mA cm −2 for 16 days under O 2 atmosphere. This excellent electrochemical performance is attributed to the high catalytic activity and abundant macro-pores of our home-made CoO. This strategy of designing CoO might be a feasible way to obtain the Li–O 2 cell with low polarization and high capacity.
研究领域:
能源材料
·
电化学
·
催化
·
电池技术
✓ 已验证
DOI
高影响因子
Nature Protocols
·
2026
·
IF 18.4
Zhang Yingying,Wu Yingnan,Jing Zehao,Chen Xiaoqiang,Li Mingle,Peng Xiaojun
Photodynamic therapy using an appropriate photocatalyst results in the production of cytotoxic reactive oxygen species for tumor ablation. However, the inherent O 2 dependence of conventional photodynamic therapy limits its clinical translation. To overcome this challenge, here we developed a selenium-substituted Nile blue derivative (ENBSe) as a versatile O 2 -independent photocatalyst. Under near-infrared light irradiation, ENBSe can drive the biological oxidation of NADH to NAD + while simultaneously triggering the cascade reduction of cytochrome c (Fe³⁺ to Fe²⁺), even in the absence of O 2 . To improve tumor specificity and targeting, we further developed a conditionally activatable photoredox catalysis (ConAPC) system. ENBSe is covalently attached to 4-nitrobenzyl chloride via a carbonic anhydride bond, wherein the nitro group can be specifically cleaved by nitroreductase (NTR), an enzyme overexpressed in hypoxic tissues. Such ConAPC design prevents reaction with NADH and quenches the fluorescences of ENBSe, which means that the drug molecule, ENBSe–NTR, is catalytically inactive. ENBSe–NTR is, to our knowledge, the first tumor microenvironment-responsive ConAPC molecule that enables O 2 -free, tumor-specific catalytic therapy. By replacing the 4-nitrobenzyl chloride group, it might be possible to target cells with different microenvironmental conditions. This protocol presents a standardized workflow encompassing the synthesis of ENBSe and its application for photocatalytic modulation of cellular electron flow in the mitochondrial electron transport chain via an O 2 -independent mechanism of action. The outlined protocol specifies a synthesis period of ~4 d for ENBSe, ~4 h for photoredox spectroscopic characterization and 4–5 weeks for photodiagnostic assessment in cancer cell and mice models.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Ge Zhang,Zhengyi Qian,Ya Mao,Baoyu Sun,Pengjian Zuo,Yulin Ma,Chunyu Du,Geping Yin,Jingying Xie
Porous carbon materials are usually employed as cathode catalysts in Li-O 2 batteries. However, the poor catalytic performance of carbon cathode often results in low capacity and severe overpotential. Herein, we successfully prepared phosphorus doped carbon material by one-step pyrolyzation, effectively improving the performance of Li-O 2 batteries. The discharge capacity of Li-O 2 battery with P doped carbon reaches 3400 m Ah g −1 at 200 mA g −1 , which is increased by 52% compared to the un-doped sample. Besides, greatly decreased discharge overpotential and enhanced rate capability are also obtained after phosphorus doping. Furtherly, phosphorus doping was found to crucially affect the growth of discharge products, and the solution driven mechanism becomes more prominent, leading to larger sized discharge products and prolonged battery life. Our work provides a new way of improving the catalytic performance of carbon cathode for Li-O 2 batteries.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2019
·
IF 15.548
Shu-qi Yang,Peng-bo Wang,Han-xin Wei,Lin-bo Tang,Xia-hui Zhang,Zhen-jiang He,Yun-jiao Li,Hui Tong,Jun-chao Zheng
Li-rich Mn-based cathode materials are regarded as promising cathode materials for Li-ion batteries (LIBs) owing to their high electrochemical capacity and low cost. However, residual Li compounds on the surface and dissolution of metal ions cause severe degradation of the electrochemical performance, thereby hindering their practical applications. Li 4 V 2 Mn(PO 4 ) 4 is a composite cathode material with three-dimensional Li-ion diffusion channels and a stable structure at high operating voltages (>4.5 V). Herein, we modify the surface of Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 with Li 4 V 2 Mn(PO 4 ) 4 . The Li 4 V 2 Mn(PO 4 ) 4 coating layer can not only reduce the content of residual Li compounds on the surface but also restrain the dissolution of transition metals. Theoretical calculations illustrate that Li 4 V 2 Mn(PO 4 ) 4 reduces the Li-ion diffusion energy barrier and provides efficient diffusion pathways. Li[Li 0.2 Mn 0.54 Ni 0.13 Co 0.13 ]O 2 @Li 4 V 2 Mn(PO 4 ) 4 compounds deliver a discharge capacity of 300 mAh g −1 with a high initial coulombic efficiency (84.2%) and an excellent cycling stability (capacity retention of 78.1% after 200 cycles at 1C). Hence, the proposed modification strategy of phosphate-based materials could shed light on the structural design of surface-sensitive electrode materials for LIBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Muhammad Mushtaq,Xianwei Guo,Yinzhong Wang,Liangwei Hao,Zhiyuan Lin,Haijun Yu
The Li–O2 battery based on the polymer electrolyte has been considered as the feasible solution to the safety issue derived from the liquid electrolyte. However, the practical application of the polymer electrolyte-based Li–O2 battery is impeded by the poor cyclability and unsatisfactory energy efficiency caused by the structure of the porous cathode. Herein, an architecture of a composite cathode with improved oxidation kinetics of discharge products was designed by an in situ method through the polymerization of the electrolyte precursor for the polymer-based Li–O2 battery. The composite cathode can provide sufficient gas diffusion channels, abundant reaction active sites, and continuous pathways for ion diffusion and electron transport. Furthermore, the oxidation kinetics of nanosized discharge products formed in the composite cathode can be improved by hexamethylphosphoramide during the recharge process. The polymer-based Li–O2 batteries with the composite cathode demonstrate highly reversible capacity when fully charged and a long cycle lifetime under a fixed capacity with low overpotentials. Moreover, the interface contact between hexamethylphosphoramide and the Li metal can be stabilized simultaneously. Therefore, the composite cathode architecture designed in this work shows a promising application in high-performance polymer-based Li–O2 batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2016
·Vol. 26
·期 43
·7847-7860
·
IF 11.382
Hong Cheng,Jing-Yi Zhu,Shi-Ying Li,Jin-Yue Zeng,Qi Lei,Ke-Wei Chen,Chi Zhang,Xian-Zheng Zhang
Conventional oxygen-dependent photodynamic therapy (PDT) has faced severe challenges because of the non-specificity of most available photosensitizers (PSs) and the hypoxic nature of tumor tissues. Here, an O 2 self-sufficient cell-like biomimetic nanoplatform (CAT-PS-ZIF@Mem) consisting of the cancer cell membrane (Mem) and a cytoskeleton-like porous zeolitic imidazolate framework (ZIF-8) with the embedded catalase (CAT) protein molecules and Al(III) phthalocyanine chloride tetrasulfonic acid (AlPcS 4 , defined as PS) is developed. Because of the immunological response and homologous targeting abilities of the cancer cell membrane, CAT-PS-ZIF@Mem is selectively accumulated at the tumor site and taken up effectively by tumor cells after intravenous injection. After the intracellular H 2 O 2 penetration into the framework, it is catalyzed by CAT to produce O 2 at the hypoxic tumor site, facilitating the generation of toxic 1 O 2 for highly effective PDT in vivo under near-infrared irradiation. By integrating the immune escape, cell homologous recognition, and O 2 self-sufficiency, this cell-like biomimetic nanoplatform demonstrates highly specific and efficient PDT against hypoxic tumor cells with much reduced side-effect on normal tissues.
研究领域:
癌症治疗
·
纳米技术
·
生物材料
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
Scientific Reports
·
2016
·Vol. 6
·期 1
·1-8
·
IF 5.228
Cai Kedi,Yang Rui,Lang Xiaoshi,Zhang Qingguo,Wang Zhenhua,He Tieshi
Gradient Mn-La-Pt catalysts with three-layered structure of manganese dioxide (MnO 2 ), lanthanum oxide (La 2 O 3 ), and Platinum (Pt) for Li-O 2 battery are prepared in this study. The mass ratio of the catalysts is respectively 5:2:3, 4:2:4, and 3:2:5 (MnO 2 : La 2 O 3 : Pt) which is start from the side of the electrolyte. The relationship between morphology structure and electrochemical performance of gradient catalyst is investigated by energy dispersive spectrometry and constant current charge/discharge test. The Li-O 2 battery based on gradient Mn-La-Pt catalysts shows high discharge specific capacity (2707 mAh g −1 ), specific energy density (8400 Wh kg −1 ) and long cycle life (56 cycles). The improvement of the Li-O 2 battery discharge capacity is attributed to the gradient distribution of MnO 2 and Pt and the involvement of La 2 O 3 that can improve the energy density of the battery. More important, this work will also provide new ideas and methods for the research of other metal-air battery.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2022
·Vol. 16
·期 6
·8405-8410
·
IF 10.269
Cao Renfei,Cui Yangfeng,Huang Gang,Liu Wanqiang,Liu Jianwei,Zhang Xinbo
Li-O 2 batteries with extremely high specific energy density have been regarded as a kind of promising successor to current Li-ion batteries. However, the high charge overpotential for the decomposition of Li 2 O 2 discharge product reduces the energy efficiency and triggers a series of side reactions that cause the Li-O 2 batteries to have a limited lifetime. Herein, Co-doped C 3 N 4 (Co-C 3 N 4 ) photocatalysts were designed by an in situ thermal evaporation method to take advantage of the photo-assisted charging technology to conquer the shortcomings of Li-O 2 batteries encountered in the charge process. Different from the commonly used photocatalysts, the Co-C 3 N 4 photocatalysts perform well no matter with and without illumination, owing to the Co doping induced conductivity and electrocatalytic ability enhancement. This makes the Co-C 3 N 4 reduce the charge and discharge overpotentials and improve the cycling performance of Li-O 2 batteries (from 20 to 106 cycles) without illumination. While introducing illumination, the performance can be further improved: Charge voltage reduces to 3.3 V, and the energy efficiency increases to 84.84%, indicating that the Co-C 3 N 4 could behave as a suitable photocathode for Li-O 2 batteries. Besides, the low charge voltage and the continuous illumination together weaken the corrosion of the Li anode, making the long-term high-efficiency operation of Li-O 2 batteries no longer just extravagant hope.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2016
·
IF 4.758
Shan Huang,Zhichun Si,Xuankun Li,Jinshuo Zou,Youwei Yao,Duan Weng
Au nanoparticles and reduced graphene oxide (r-GO) co-modified TiO 2 nanotube arrays (TNTs) were prepared by a facile and green strategy based on the electro-deposition technology for detecting H 2 O 2 , O 2 and nitrite. As-prepared Au/r-GO/TNTs electrode was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). The results clearly demonstrate that the successful attachment of r-GO sheets and narrow-range distribution of Au nanoparticles on TNTs . The reduced grapheme oxide sheet can help to improve the electronic conductive performance of TNTs and prevent the agglomeration of Au nanoparticles. Electrochemical studies reveal that the Au/r-GO/TNTs electrode exhibit excellent electrocatalytic performance toward the reduction of H 2 O 2 . Under the optimal experimental condition, the sensor has a quick response to H 2 O 2 at −0.3 V with a high sensitivity (1011.35 mA M −1 cm −2 ), wide linear range (0.01–22.3 mM) and low detection limit (0.006 μM). In addition, the sensor also has good stability and excellent selectivity. Moreover, the established Au/r-GO/TNTs electrode also shows high sensitivities towards dissolved O 2 and nitrite ions, which has great potential for the development of electrochemical sensors, molecular bioelectronics devices and biosensors.
研究领域:
生物传感器
·
电化学检测
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）