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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Engineering oxygen vacancies in Co3O4 to boost p-d hybridization for hydrogeneration of nitrogen and oxygen

Xianwei Li,Shuangxiu Ma,Fang Luo,Zehui Yang

Electrochemical hydrogenerations of nitrogen and oxygen molecules are of significance for nitrogen reduction and oxygen reduction reactions. Strengthening the binding between active sites and gaseous molecules is beneficial for enhancing the catalytic performance, especially in NRR catalysis. In this work, we have engineered the oxygen vacancies in Co 3 O 4 nanoparticles to boost the catalytic activity towards NRR and ORR. Ascribing to the p-d hybridization between Co and N atoms, N 2 electrochemical adsorption is promoted and the related energy barrier of N 2 protonation is significantly decreased by 50%; as a consequence, Faradaic efficiency is 11.2% at −0.4 V vs. RHE, 3-fold higher than Co 3 O 4 /CNT; moreover, due to the oxygen vacancies in Co 3 O 4-x /CNT leading to a higher oxophilicity, Co 3 O 4-x /CNT showed a better selectivity in ORR catalysis and kinetic current density at 0.85 V vs. RHE is boosted by 2.4 times. Consequently, Co 3 O 4-x /CNT exhibits a better rechargeable zinc air battery performance than Pt/C-IrO 2 by a factor of 2.2.

研究领域: 材料科学 · 电化学 · 催化科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2025 · IF 3.7

Multifunctional High-Entropy Alloys and Oxides for Self-Powered Electrocatalytic Nitrate Reduction to Ammonia

Quan Zhang,Shiming Qiu,Lehua Wang,Kang Lian,Jun Luo,Xijun Liu

Graphical High-entropy alloys (HEAs) and high-entropy alloy oxides (HEOs) are considered as promising ORR and NO 3 − RR candidates. By FeNiCoMnRh/NC assembled ZAB coupled to drive NO 3 − RR system (FeNiCoMnCuO x /NC as a cathode), which provides an attractive route for low-energy sewage treatment and environmentally friendly preparation of ammonia. High-entropy alloys (HEAs) show high activities toward oxygen reduction reaction (ORR), Zn-air batteries (ZABs) and nitrate reduction reaction (NO 3 − RR). In this work, FeNiCoMnRh HEA supported by N-doped carbon frameworks is prepared and showed excellent ORR performance with a half-wave potential ( E 1/2 ) of 0.89 V versus RHE, limiting diffusion current ( j L ) of 5.6 mA cm −2 and better current stability. The HEA-assembled ZAB exhibited a high-power density of 103.8 mW cm −2 with a specific capacity of 790 mAh g Zn −1 . Also, its oxides presented 77% Faraday efficiency (FE) for ammonia production at −0.3 V versus RHE. Accordingly, our designed ZAB was employed to drive NO 3 − RR to construct a self-powered system, which provides an attractive route for low-energy sewage treatment and environmentally friendly preparation of ammonia.

研究领域: 材料科学 · 环境科学 · 电催化
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ChemElectroChem · 2017 ·Vol. 5 ·期 3 ·471-477 · IF 4.136

Fe/Fe3C Nanoparticles Embedded in Nitrogen-Doped Carbon Nanotubes as Multifunctional Electrocatalysts for Oxygen Catalysis and CO2 Reduction

Jingchun Jia,Huijuan Yang,Genxiang Wang,Peng Huang,Pingwei Cai,Zhenhai Wen

Graphical All-round activity : Hybrids of Fe/Fe 3 C embedded in N-doped carbon nanotubes (Fe/Fe 3 C@NCNTs) are prepared by pyrolyzing mixtures of Fe 3 O 4 nanoparticles and dicyandiamide. Fe/Fe 3 C@NCNTs show a highly multifunctional catalytic activity for the oxygen evolution, oxygen reduction, and CO 2 reduction reactions. Hybrids of Fe/Fe 3 C embedded in N-doped carbon nanotubes (Fe/Fe 3 C@NCNTs) are prepared by pyrolyzing mixtures of Fe 3 O 4 nanoparticles and dicyandiamide. The systematic electrochemical study of Fe/Fe 3 C@NCNTs shows a decent catalytic activity toward the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). The sample of Fe/Fe 3 C@NCNTs at 750 °C exhibits a remarkably high activity with an onset potential of 1.47 V for the OER, and an onset potential of 0.96 V and half-wave potential 0.88 V for the ORR, which inspired us to set up a rechargeable Zn-air battery with such Fe/Fe 3 C@NCNT nanohybrids as the cathode materials, showing a maximum power density of 198 mW cm −2 and long-term stability after 500 cycles. We also demonstrate that Fe/Fe 3 C@NCNTs present favorable electrocatalytic activity towards the CO 2 reduction reaction (CO 2 RR) with a low onset potential and good selectivity. The major products are a mixture of H 2 and CO gases that can be used for methanol production in the Fischer−Tropsch process.

研究领域: 材料科学 · 电化学 · 能源科学
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Small · 2018 ·Vol. 14 ·期 8 ·1702827 · IF 9.598

A Bifunctional Highly Efficient FeNx/C Electrocatalyst

Erling Li,Fa Yang,Zhemin Wu,Yong Wang,Mingbo Ruan,Ping Song,Wei Xing,Weilin Xu

Herein, a type of Fe, N-codoped carbon electrocatalyst (FeN x /C, Fe-N-BCNT#BP) containing bamboo carbon nanotubes and displaying bifunctional high catalytic efficiency for both oxygen reduction reaction (ORR) and carbon dioxide reduction reaction (CO2RR) is reported. It shows high electrocatalytic activity and stability for both the ORR process with onset potential of 1.03 V RHE in alkaline and the CO2RR to CO with high faradic efficiency up to 90% and selectivity of about 100% at low overpotential of 0.49 V. For CO2RR to CO, it is revealed that Fe 3 C is active but the activity of FeN x centers is lower than that of C–N-based centers, contrary with that observed for ORR. Due to its low cost and high electrocatalytic performance for these two reduction reactions, the obtained catalyst is very promising for extensive application in future. The revealed huge activity difference of the same types of active sites for different reactions can efficiently guide the synthesis of advanced materials with multifunction.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Efficient Tetra-Functional Electrocatalyst with Synergetic Effect of Different Active Sites for Multi-Model Energy Conversion and Storage

Sobia Dilpazir,Pengju Ren,Rongji Liu,Menglei Yuan,Muhammad Imran,Zhanjun Liu,Yongbing Xie,He Zhao,Yijun Yang,Xi Wang,Carsten Streb,Guangjin Zhang

Energy crisis and global warming due to excessive CO2 emissions are the two major challenges of the world. Conversion of CO2 into useful fuels along with rechargeable metal air batteries and water splitting is one way to combat the energy crisis, which is bottlenecked due to the lack of multifunctional electrocatalyst. Herein simple but multifunctional electrocatalyst, which combined CoNi nanoalloy, N-doped carbon nanotubes, and single atomic Ni sites together is reported. The prepared electrocatalyst has shown remarkable performance for CO2RR, ORR, OER, and HER. The practical utilization of the catalyst is mansifested by a dual model metal CO2/air battery and water electrolyzer. An excellent CO2RR with FE of 99% is achieved in 0.5 M KHCO3 medium. The catalyst exhibits more positive onset (0.98 V) and half wave potential (0.86 V) than Pt/C for ORR, extremely low overpotential (η10) of 250 mV for OER, and thus the lowest ORR/OER potential gap of 0.62 V. In alkaline medium, the catalyst also shows excellent HER performance with η10 of 49 mV, resulting in the smallest cell bias of 1.57 V for overall water splitting to date. This work provides a new pathway to design more stellar multifunctional electrocatalyst for sustainable and clean renewable energy technology.

研究领域: 材料科学 · 能源技术 · 催化化学
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CHEMOSPHERE · 2023 · IF 8.8

A novel flow-through dual-system electro-Fenton for boosting PAEs removal efficiency in natural waters

Bei Wu,Zhiqiang Jiang,Weidong Lei,Jie Sun,Zhi Chen

In a conventional electro-Fenton system with a single cathode, it is difficult to attain both high H 2 O 2 generation by oxygen reduction reaction (ORR) and efficient iron reduction reaction (FRR). For this study, a flow-through dual-system electro-Fenton (FT-DEF) reactor was designed to overcome this shortcoming and promote mass transfer to effectively remove dimethyl phthalate (DMP) from water. By comparing the ORR and FRR performances of four different commercial carbon electrodes, the graphite felt with the highest amount of H 2 O 2 generation was selected as the cathode of the ORR system, and the activated carbon fiber with the best Fe (III) reduction effect was selected as another cathode of the FRR system. The ORR system and FRR system operate simultaneously to form the DEF system. The FT-DEF system displayed many advantages compared with the conventional electro-Fenton (CI-ORR), presenting an improved efficiency and low energy consumption in phthalates removal. Under optimal reaction conditions, the FT-DEF system is capable to degrade 100% DMP in 20 min, which is 25% higher than the CI-ORR, while the reaction rate constant (0.271 min −1 ) is 16 times that of CI-ORR system (0.017min −1 ). In addition, the TOC removal of FT-DEF achieving 72.3% within 2 h with energy consumption of 2.35 kW h·m −3 is much better than CI-ORR that only achieves 18.3% TOC removal within 2 h with energy consumption of 8.13 kW h·m −3 . Furthermore, control parameters and mechanism of FT-DEF were investigated in detail. The main intermediate products of DMP were analyzed by UPLC-ESI-HRMS, and the possible degradation path of DMP was speculated. In addition, application of FT-DEF in three types of natural water demonstrated its universal applicability of the system.

研究领域: 环境科学 · 化学工程
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Materials · 2020 ·Vol. 13 ·期 20 ·4551 · IF 3.057

Facile Synthesis of the Amorphous Carbon Coated Fe-N-C Nanocatalyst with Efficient Activity for Oxygen Reduction Reaction in Acidic and Alkaline Media

Linglei Jin,Baikang Zhu,Xuesong Wang,Le Zhang,Debin Song,Jian Guo,Hengcong Tao

With the assistance of surfactant, Fe nanoparticles are supported ong-C3N4nanosheets by a simple one-step calcination strategy. Meanwhile, a layer of amorphous carbon is coated on the surface of Fe nanoparticles during calcination. Transmission electron microscopy (TEM), scanning electron microscope (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma (ICP) were used to characterize the morphology, structure, and composition of the catalysts. By electrochemical evaluate methods, such as linear sweep voltammetry (LSV) and cyclic voltammetry (CV), it can be found that Fe25-N-C-800 (calcinated in 800 °C, Fe loading content is 5.35 wt.%) exhibits excellent oxygen reduction reaction (ORR) activity and selectivity. In 0.1 M KOH (potassium hydroxide solution), compared with the 20 wt.% Pt/C, Fe25-N-C-800 performs larger onset potential (0.925 V versus the reversible hydrogen electrode (RHE)) and half-wave potential (0.864 V vs. RHE) and limits current density (2.90 mA cm−2, at 400 rpm). In 0.1 M HClO4, it also exhibits comparable activity. Furthermore, the Fe25-N-C-800 displays more excellent stability and methanol tolerance than Pt/C. Therefore, due to convenience synthesis strategy and excellent catalytic activity, the Fe25-N-C-800 will adapt to a suitable candidate for non-noble metal ORR catalyst in fuel cells.Keywords:oxygen reduction reaction;iron;coating;P-123

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Nitrogen, Sulfur Co-Doped Hierarchically Porous Carbon as a Metal-Free Electrocatalyst for Oxygen Reduction and Carbon Dioxide Reduction Reaction

Ruru Li,Feng Liu,Yihao Zhang,Mingming Guo,Dong Liu

High-cost and low-efficiency electrocatalysts have hindered oxygen reduction reaction (ORR) in fuel cells and CO2 reduction reaction (CO2RR) for producing fuels and value-added chemicals. Here, a low-cost metal-free electrocatalyst of a N, S co-doped hierarchically porous carbon (NSHPC) for efficient ORR and CO2RR is reported. The NSHPC is prepared by pyrolysis of glucosamine hydrochloride and thiocyanuric acid precursors using SiO2 as hard templates. The N, S co-doping effectively enhances catalytic activity and selectivity, and the hierarchically porous structure largely exposes abundant active sites to reaction species and facilitates electrolyte transport, thereby leading to significantly increased catalytic activities for the NSHPC. The resultant NSHPC exhibits excellent electrocatalytic activities toward ORR in both acidic and alkaline electrolytes and also shows application in proton exchange membrane fuel cells (PEMFCs). More importantly, the NSHPC enables CO2 reduction to CO with 87.8% maximum Faraday efficiency (FE) in aqueous electrolytes. This work offers a novel insight into the development of multifunctional electrocatalysts for producing electricity, fuels, and value-added chemicals.

研究领域: 材料科学 · 电化学 · 能源科学
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NEW CARBON MATERIALS · 2025 · IF 6.8

The synthesis of electrospun N-doped carbon nanofibers with embedded Fe2N/Fe3C species for catalyzing the O2 and CO2 reduction reactions

Xiu-zhen LV,Xiang-xiang XU,Meng-meng YU,Yi-chen WEI,Jun-ying WANG,Jun-zhong WANG

The need for bi-functional catalysts that facilitate both the oxygen reduction (ORR) and carbon dioxide reduction (CO 2 RR) reactions arises from their potential to help solve the critical problems of carbon neutrality and renewable energy conversion. However, there are few reports on the development of bi-functional catalysts for zinc-air battery-driven CO 2 RR devices. We introduce a novel approach for synthesizing Fe 2 N/Fe 3 C species embedded in nitrogen-doped carbon nanofibers by electrospinning a solution of Hemin and polyacrylonitrile in N,N-dimethylformamide. The material has an exceptional catalytic performance, with a half-wave potential of 0.91 V versus RHE for the ORR and values of over 90% for both the selectivity and Faradaic efficiency for the CO 2 RR. The high catalytic performances are attributed to the strong coupling between the Fe 3 C/Fe 2 N heterostructure and the Fe-N-C sites in the nitrogen-doped carbon nanofibers. Notably, both Fe 3 C and Fe 2 N play distinct roles in both the ORR and CO 2 RR. This investigation indicates a way for designing advanced carbon-based bi-functional catalysts for use in this field. Download: Download high-res image (61KB) Download: Download full-size image

CAS / MDL: 68-12-2
研究领域: 材料科学 · 电化学 · 可再生能源
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2022 ·Vol. 23 ·期 20 ·12679 · IF 6.208

Zn-Catalyzed Regioselective and Chemoselective Reduction of Aldehydes, Ketones and Imines

Miaomiao Zhang,Hongmei Jiao,Haojie Ma,Ran Li,Bo Han,Yuqi Zhang,Jijiang Wang

An operationally convenient Zn-catalyzed synthesis of alcohols by the reduction of aldehydes, ketones, andα,β-unsaturated aldehydes/ketones is reported. It is a rare example of using mild and sustainable HBpin as a reductant for catalytic reduction of carbonyl compounds in the absence of acid or base as hydrolysis reagent. The reaction is upscalable and proceeds in high selectivity without the formation of boronate ester by-products, and tolerates sensitive functionalities, such as iodo, bromo, chloro, fluoro, nitro, trifluoromethyl, aminomethyl, alkynyl, and amide. The Zn(OAc)2/HBpin combination has been also proved to be chemoselective for the C=N reduction of imine analogs.Keywords:zinc;reduction;aldehydes;ketones;imines

CAS / MDL: 7758-94-3
研究领域: 有机化学 · 合成化学
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INORGANIC CHEMISTRY · 2025 · IF 4.7

Mechanistic Insights into Molybdenum–Iron-Catalyzed Neptunium Reduction and Extraction

Huaixin Hao,Yuxiao Guo,Bin Li,Qilong Tang,Yaoyang Liu,Xue Dong,Chao Xu,Jing Chen,Zhipeng Wang

Neptunium (Np), as a critically regarded actinide in nuclear waste, is of great significance for environmental hazard mitigation and the resource-oriented management of nuclear waste. The reduction of Np(V) to Np(IV) represents a pivotal step toward efficient Np recovery. However, this process is profoundly influenced by the intricate redox chemistry of Np itself and the diverse concomitant fission products in spent nuclear fuel, with the underlying mechanistic details remaining inadequately elucidated. In this study, we demonstrated that molybdenum (Mo) and iron (Fe) dramatically accelerated the reduction rate of Np(V) by approximately 2 × 104-fold. Additionally, by integrating analytical techniques including absorption spectroscopy, stopped-flow spectroscopy, inductively coupled plasma–mass spectrometry, and solvent extraction, we deciphered the electron transfer interactions between Mo and Fe, as well as their synergistic catalytic mechanism in driving the Np(V)–Np(IV) conversion. This study not only advances the fundamental understanding of Np redox chemistry in complex nuclear waste matrices but also offers technical support for optimizing nuclear waste treatment protocols.

CAS / MDL: 50-81-7 540-72-7
研究领域: 核化学 · 环境科学
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Materials Horizons · 2017 ·Vol. 5 ·期 1 ·108-115 · IF 10.706

Co/CoP embedded in a hairy nitrogen-doped carbon polyhedron as an advanced tri-functional electrocatalyst

Yongchao Hao,Yuqi Xu,Wen Liu,Xiaoming Sun

The design and synthesis of a multi-functional electrocatalyst with low cost and high efficiency is still a great challenge. Herein, we report the rational design and realization of a tri-functional electrocatalyst featuring Co/CoP embedded in a hairy nitrogen-doped carbon polyhedral (Co/CoP–HNC) derived from common metal organic frameworks (MOFs). The components of Co, CoP, and hairy nitrogen-doped carbon in the catalyst respectively render catalytic activity, high electrochemical surface area, and electronic conductivity. The synergy of the tailored Co/CoP–HNC catalyst provides high activity for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The catalytic performance and assembly feasibility are further demonstrated in overall water splitting and Zn–air battery tests, and both revealed high efficiency and long durability of the proposed electrocatalyst.

研究领域: 材料科学 · 能源化学 · 催化化学
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