Journal of Energy Chemistry
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2022
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IF 13.599
Rong Li,Jiale Ding,Xijiao Mu,Yifei Kang,Anran Wang,Weihui Bi,Yunhe Zhang,Jing Cao,Qingfeng Dong
The extreme instability of pure α-phase FAPbI 3 under high humidity conditions restricts the high-throughput fabrication in unmodified air environments, resulting in poor performance of α-phase FAPbI 3 perovskite devices obtained by scalable fabrication methods. Here we synthesized hyperbranched copper phthalocyanine (HCuPc) as a supramolecular additive with twisted phthalocyanine units to realize the molecular-level encapsulation at the grain boundaries through supramolecular interaction, which greatly broadened the processing window of FAPbI 3 under high humidity. At the same time, unlike traditional encapsulation layer that carrier can only be collected by tunneling effect, the twisted phthalocyanine ring of HCuPc in perovskite films is more conducive to hole extraction. Finally, a record efficiency was achieved in pure FAPbI 3 based inverted structured solar cell by blade-coating to the best of our knowledge, even under unmodified humid air conditions (relative humidity of 65%–85%). The best operational stability of 3D pure FAPbI 3 devices can also be achieved at the same time and unencapsulated HCuPc-FAPbI 3 device can even operate with negligible degradation for 100 h in the open air (RH 30%–40%).
研究领域:
材料科学
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纳米科技
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能源化学
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光伏技术
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表面与界面化学
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GREEN CHEMISTRY
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2026
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IF 10.6
Wujiao Tan,Wenhao Yang,Dan You,Yiwei Yu,Ao Yan,Li Zhang,Xue Li,Ziyi Zhu,Yiyong Zhang
Aqueous zinc-ion batteries present several advantages, including high safety and low cost. However, severe dendrite growth and side reactions at the zinc anode significantly impede their cycle life and efficiency. This study proposes a zinc deposition regulation strategy based on a synergistic “chelation-relay” mechanism achieved by constructing a phthalocyanine functional layer on the surface of a cellulose separator. The phthalocyanine layer, which is rich in nitrogen coordination centers, effectively chelates Zn2+, reshaping the electrode/electrolyte interface structure and inhibiting side reactions. Its macrocyclic conjugated architecture functions as an “ion relay”, facilitating reversible storage and providing ordered migration channels for Zn2+, thereby alleviating concentration polarization and promoting uniform deposition. COMSOL simulation results demonstrate that this functional layer can homogenize the interfacial electric field and Zn2+ flux, thereby suppressing the “tip effect” associated with dendrite formation. Consequently, stable zinc deposition and stripping over 1000 cycles under conditions of 1 mA cm−2 and 1 mAh cm−2 yield an average coulombic efficiency of 99.1%. Furthermore, the Zn/I2 full cell exhibits a capacity retention rate of 98.83% after 10 000 cycles at a discharge rate of 1 A g−1. These findings underscore the potential of phthalocyanine to regulate zinc deposition, contributing to the development of high-performance aqueous zinc-ion batteries.
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Nature Communications
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2026
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IF 18.1
Qi Shi-Chao,Han Yan-Yan,Liu Yong-Lan,Zhao Yun-Jie,Huang Qi-Qi,Liu Xiao-Qin,Sun Lin-Bing
Traditionally, adsorption is believed to take place only in the ground state, but here we report an excitation-driven adsorption mode. Composites of metallophthalocyanines and carbonaceous substrates are prepared, among which the potassium-phthalocyanine (KPc)/reduced graphene oxide (RG) composite shows the most typical behavior. Femtosecond transient absorption spectroscopy and first-principles simulations reveal that under ultraviolet (UV) irradiation, the excited electrons in the composite transfer efficiently from KPc to RG, leaving long-lived excited holes on KPc that enable selective adsorption of CO molecules. In the dark, the composite shows negligible CO adsorption (0.06 mmol g⁻ 1 ), whereas its CO uptake increases to 1.20 mmol g⁻ 1 upon UV light, with a UV-modulated adsorption capacity ratio of up to 95%. This adsorption mode is also applicable to other metallophthalocyanine/carbonaceous composites. This work presents a potential strategy for photoexcitation utilization and the development of energy-efficient chemical separation technologies.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Yangke Long,Shixin Huang,Jianlin Sun,Dan Peng,Zuotai Zhang
Highly dispersed iron nanoclusters on carbon (FeNC@C) hold great promise for wastewater purification in Fenton-like reactions. The microenvironment engineering of central Fe atom is promising to boost the activation capacity of FeNC@C, which is however remains a challenge. This study developed a self-sacrificed templating strategy to S, N-codoped carbon supported Fe nanoclusters (FeNC@SNC) activator and find the key role of sulfur heteroatoms in regulating the electron structure of Fe sites and final activation property. Investigations revealed that the FeNC@SNC composite exhibited unusual bifunctional activity in both peroxymonosulfate (PMS)- and periodate (PI)-based Fenton-like reactions. We also offered insights into the differences between the degradation of organics by the FeNC@SNC/PMS and FeNC@SNC/PI systems. Specifically, under identical conditions, the FeNC@SNC/PMS system delivered a higher oxidation capability and stronger resistance to nontarget matrix constituents, but showed more severe Fe leaching than the FeNC@SNC/PI system. Furthermore, while mediated electron-transfer process was identified as the major route for pollutant decomposition in both systems, the high-valent Fe-oxo species [Fe (IV)] was the auxiliary reactive species found only in the FeNC@SNC/PMS system. Based on these findings, our results provide profound insights into the design of active and durable Fe-based activators toward highly efficient Fenton-like reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Menghui Chen,Yongting Chen,Jialin Cai,Zhili Yang,Meihua Tang,Joey Chung-Yen Jung,Shengli Chen,Jiujun Zhang,Shiming Zhang
Revealing the types of and interplays among multiple active-sites in iron-nitrogen-carbon (Fe N C) materials is of great significance for developing high-performance, Fe-based non-precious metal catalysts for oxygen reduction reaction (ORR). In this paper, a single-atom Fe N C catalyst is prepared through high-temperature pyrolyzing of melamine foam (MF), iron phthalocyanine (FePc), phthalocyanine (Pc), and zinc (Zn)-salts composite. The catalyst is found to contain a variety of active-sites, including carbon atom next to pyridinic-N (pyridinic N C), Fe-N 4 and pore defect. It is shown that MF with high N -content is responsible for the formation of the main pyridinic N C sites and in the meantime acts as the self-sacrificed template for framework of the catalyst. The presence of Pc can facilitate the formation of the predominant Fe-N 4 sites, since the interplay between Pc and FePc results in a confinement of Fe-N 4 . Zn-salts serve as the pore-forming additives to create sufficient pore defects which can also anchor pyridinic N C and Fe-N 4 structures. The results of density functional theory (DFT) calculations suggest that the multiple active-sites function synergistically to enable high-efficiency ORR electrocatalysis. The optimal Fe N C catalyst shows superior ORR activity with a half-wave potential of ∼0.88 V ( vs . RHE), as well as high methanol tolerance and electrochemical stability compared to the commercial carbon-supported platinum (Pt/C) catalyst.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Yueqi Li,Minjuan Cai,Bingbing Ji,Feng Wu,Li-Zhi Huang
Carbonous materials were found to catalyze the dechlorination of trichloroethylene (TCE) by green rust (GR), but the catalytic mechanism was not fully understood. We have developed a facile ball milling method to synthesize N-doped graphene (NG) with various N species, catalyzing fast dechlorination of TCE to acetylene by GR with the highest acetylene production rate of ~0.1 d −1 . The adsorption of TCE onto NG is mainly derived from the graphene region of NG, and high pyridinic N is essential for the enhanced TCE reduction by GR. Oxygen species did not enhance the TCE reduction in GR/NG system. High dechlorination rates are correlated to a high amount of defect in NG and a high electron conductivity of NG. Pyridinic N has the highest adsorption energy for TCE among all the N species, which leads to the highest catalytic performance. High electrochemically active surface area resulted from the high content of pyridinic N facilitate the NG-catalyzed dechlorination. The acetylene production rate in real groundwater is still around one-third of that in ultrapure water. This work not only reveals the catalytic mechanism of NG-catalyzed dechlorination by GR, but also provide a feasible approach for practical remediations of TCE-contaminated groundwater using GR-NG mixture.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Kejun Chen,Maoqi Cao,Ganghai Ni,Shanyong Chen,Hanxiao Liao,Li Zhu,Hongmei Li,Junwei Fu,Junhua Hu,Emiliano Cortés,Min Liu
Nickel phthalocyanine (NiPc) can be at first glance a compelling catalyst for CO 2 reduction reaction (CO 2 RR) because of its Ni–N 4 site. Unfortunately, the pristine NiPc possesses a low catalytic activity resulting from the poor CO 2 adsorption and activation capabilities of the electron-deficiency Ni site. Herein, we develop nickel polyphthalocyanine (NiPPc) with extended conjugation to tailor the electronic density at the Ni active site. The enlarged π conjugation of NiPPc evokes the d-electrons localization, increasing the electronic density at the Ni site, which enhances its CO 2 adsorption and activation. Consequently, NiPPc supported on carbon nanotubes (NiPPc/CNT) in a flow cell delivers an excellent activity of −300 mA cm −2 for CO 2 RR with the CO selectivity of 99.8%, which is much higher than that of NiPc dispersed on carbon nanotubes. NiPPc/CNT exhibits an outstanding stability for CO 2 RR of more than 30 h at a current density of −100 mA cm −2 with an ultrahigh selectivity for CO, exceeding 99.7%. This work showcases a new way of tuning the electronic density of catalytic sites.
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MOLECULES
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2021
·Vol. 26
·期 24
·7537
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IF 4.412
Yilin Huang,Weidong Xue,Xingwang Hou,Rui Zhao
In this paper, we will discuss the excellent broadband microwave absorption behaviors of Cu/CuO/carbon nanosheet composites: traces of copper and oxide embedded in a carbon nano-sheet not only cut down the high permittivity of adsorbs but also induce more interfacial polarization centers. The results showed that at a cracking temperature of 900 °C, the fabricated material has a unique ripple-like structure, which promotes the hierarchical interfacial polarization. The prepared material has a maximum absorption bandwidth of 4.48 GHz at an exceedingly thin thickness of 1.7 mm and a maximum reflection loss of −25.3 dB at a thickness of 2 mm. It is a relatively ideal material for electromagnetic wave absorption.Keywords:metal phthalocyanine;carbon nanosheet;solid-state pyrolysis;electromagnetic wave absorption
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高影响因子
Nature Communications
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2023
·Vol. 14
·期 1
·1-12
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IF 16.6
Cao Peike,Quan Xie,Nie Xiaowa,Zhao Kun,Liu Yanming,Chen Shuo,Yu Hongtao,Chen Jingguang G.
Direct hydrogen peroxide (H 2 O 2 ) electrosynthesis via the two-electron oxygen reduction reaction is a sustainable alternative to the traditional energy-intensive anthraquinone technology. However, high-performance and scalable electrocatalysts with industrial-relevant production rates remain to be challenging, partially due to insufficient atomic level understanding in catalyst design. Here we utilize theoretical approaches to identify transition-metal single-site catalysts for two-electron oxygen reduction using the *OOH binding energy as a descriptor. The theoretical predictions are then used as guidance to synthesize the desired cobalt single-site catalyst with a O-modified Co-(pyrrolic N) 4 configuration that can achieve industrial-relevant current densities up to 300 mA cm − 2 with 96–100% Faradaic efficiencies for H 2 O 2 production at a record rate of 11,527 mmol h − 1 g cat − 1 . Here, we show the feasibility and versatility of metal single-site catalyst design using various commercial carbon and cobalt phthalocyanine as starting materials and the high applicability for H 2 O 2 electrosynthesis in acidic, neutral and alkaline electrolytes.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Yangke Long,Jian Dai,Shiyin Zhao,Yiping Su,Zhongying Wang,Zuotai Zhang
Pollutant degradation via periodate (IO4–)-based advanced oxidation processes (AOPs) provides an economical, energy-efficient way for sustainable pollution control. Although single-atomic metal activation (SMA) can be exploited to optimize the pollution degradation process and understand the associated mechanisms governing IO4–-based AOPs, studies on this topic are rare. Herein, we demonstrated the first instance of using SMA for IO4– analysis by employing atomically dispersed Co active sites supported by N-doped graphene (N-rGO-CoSA) activators. N-rGO-CoSA efficiently activated IO4– for organic pollutant degradation over a wide pH range without producing radical species. The IO4– species underwent stoichiometric decomposition to generate the iodate (IO3–) species. Whereas Co2+ and Co3O4 could not drive IO4– activation; the Co–N coordination sites exhibited high activation efficiency. The conductive graphene matrix reduced the contaminants/electron transport distance/resistance for these oxidation reactions and boosted the activation capacity by working in conjunction with metal centers. The N-rGO-CoSA/IO4– system exhibited a substrate-dependent reactivity that was not caused by iodyl (IO3·) radicals. Electrochemical experiments demonstrated that the N-rGO-CoSA/IO4– system decomposed organic pollutants via electron-transfer-mediated nonradical processes, where N-rGO-CoSA/periodate* metastable complexes were the predominant oxidants, thereby opening a new avenue for designing efficient IO4– activators for the selective oxidation of organic pollutants.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Qingshan Zhao,Xiaojie Tan,Tianwen Ma,Fengliang Cao,Zhengzheng Xia,Hui Liu,Hui Ning,Zhongtao Li,Han Hu,Mingbo Wu
Massive production of efficient, durable, and low-cost electrocatalysts toward oxygen reduction reaction (ORR) is urgently desired for the development of energy storage and conversion devices. In this study, a facile and cost-effective strategy is proposed for the scalable synthesis of atomically dispersed Fe N C derived from petroleum asphalt (Fe N C@PA) as a reinforced catalyst for ORR. The Fe N C@PA is fabricated through a layer-by-layer cladding template and subsequent pyrolysis method. Intercalating appropriate amount of petroleum asphalt not only improves the graphitic degree to reinforce the atomic Fe−N x active sites, but also increases mass yield of the catalyst (~220%) compared with the Fe N C counterpart. Serving as an ORR electrocatalyst, the optimized Fe N C@PA-1:4 provides almost a four-electron transfer pathway (3.96) and exhibits superior electrocatalytic activity with a half-wave potential (E 1/2 ) of 0.90 V to the commercial Pt/C catalyst (E 1/2 = 0.86 V), as well as promoted durability and methanol tolerance in alkaline medium. Moreover, the zinc-air battery based on Fe N C@PA-1:4 cathode delivers a high power density of 166.7 mW cm −2 . This work may help the massive production of robust atomically dispersed non-noble metal catalysts for ORR and provide a new avenue for the high value-added utilization of petroleum asphalt.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Xiao-Cheng Liu,Chuan-Shu He,Zi-Yang Shen,Wen-Qiang Li,Ning Chen,Jun-Sheng Song,Xiao-Guo Zhou,Yang Mu
Fe(III) chelate reduction is of great importance in the homogeneous neutral electro-Fenton (EF) process, but its reduction mechanisms with different reductive species remain unclear. In this study, the reduction mechanisms of several typical Fe(III) chelates through electron and atomic H* were investigated using experiments and density functional theory calculations. The results indicated that the electron reduction efficiencies for [Fe(III)-EDTA] − and [Fe(III)-EDDS] − chelates were 16.23 and 8.31 times higher compared to [Fe(H 2 O) 6 ] 3+ , which was featured by low E LUMO - HOMO and concentrated LUMO distribution around Fe atom. In contrast, the atomic H* reduction efficiency for [Fe(III)-HA] 3+ chelate was 10 times higher than that of electron, attributed to high chelation ability of HA and negative energy barrier of [Fe(III)-HA] 3+ reduction in the atomic H*-dominated system. Additionally, phthalocyanine (Pc) had insignificant effect on pollutant degradation efficiency in the neutral EF systems due to the lower chelate ability of Pc with Fe(III) compared to H 2 O.
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