Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 5
·124731
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IF 7.5
Nan Zhang,Menglin Gao,Wenru Cheng,Zhaocun Song,Xichen Yang
The development of efficient and cost-effective electrocatalysts for hydrogen production is crucial for advancing a carbon-neutral circular economy. The hydrogen evolution reaction (HER) performance of MoS 2 in alkaline media is hindered by its sluggish water-dissociation kinetics and inert basal planes. Herein, we report a novel ternary heterostructure, consisting of γ-FeOOH nanosheets and smaller Ni 3 S 2 nanosheets grown on vertical 1 T/2H MoS 2 nanosheets, that exhibits enhanced HER activity. Systematic investigations suggest that the enhanced HER performance is associated with the interfacial interactions among Ni 3 S 2 , γ-FeOOH, and MoS 2 , which involve strain coupling, electronic coupling, and functional synergy. Accordingly, the Ni 3 S 2 /γ-FeOOH/MoS 2 /CC electrode requires overpotentials of only 99.6 and 176.1 mV at 10 and 100 mAcm −2 , respectively. Remarkably, it outperforms commercial Pt/C at current densities exceeding 173.2mA cm −2 and requires an overpotential of only 213.9mV at 300 mA cm −2 , while also exhibiting robust operational stability at high current densities, highlighting its promise for further exploration toward practical alkaline water electrolysis systems. This work provides a promising strategy for designing high-performance, earth-abundant MoS 2 -based HER catalysts for alkaline water electrolysis.
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GREEN CHEMISTRY
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2019
·Vol. 21
·期 10
·2709-2719
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IF 9.405
Hao Tang,Ning Li,Guangyi Li,Aiqin Wang,Yu Cong,Guoliang Xu,Xiaodong Wang,Tao Zhang
For the first time, gasoline and jet fuel range C7–C8 cycloalkanes and aromatics were selectively synthesized by the alcoholysis of poly(ethylene terephthalate) (PET) waste, followed by solvent-free hydrogenation and hydrodeoxygenation (HDO). It was found that methanol is highly reactive for the alcoholysis of PET waste. In the absence of any catalyst, a high yield of dimethyl terephthalate (97.3%) was achieved under mild conditions (473 K, 3.5 h). Dimethyl terephthalate exists as a solid and can be automatically separated from methanol with a decrease in temperature. Subsequently, dimethyl terephthalate was liquefied to dimethyl cyclohexane-1,4-dicarboxylate by hydrogenation over noble metal catalysts. Among the investigated catalysts, Pt/C exhibited the highest activity. Finally, the dimethyl cyclohexane-1,4-dicarboxylate as obtained was further hydrodeoxygenated to C7–C8 cycloalkanes and aromatics that can be used as gasoline or additives to improve the densities (or volumetric heat value) and sealabilities of current bio-jet fuels. Bimetallic Ru–Cu/SiO2 was found to be a promising HDO catalyst. According to the characterization results, the excellent HDO performance of Ru–Cu/SiO2 can be explained by the formation of smaller Ru–Cu alloy particles during the catalyst preparation. In real applications, dimethyl cyclohexane-1,4-dicarboxylate can also be simultaneously hydrodeoxygenated with biomass derived oxygenates to produce jet fuel with a suitable content of cycloalkanes and aromatics.
研究领域:
化学工程
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材料科学
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环境科学
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能源
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高影响因子
FARADAY DISCUSSIONS
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2014
·Vol. 176
·393-408
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IF 4.194
Yan Xie,Chizhou Tang,Zhiqiang Hao,Yang Lv,Ruixia Yang,Xuming Wei,Weiqiao Deng,Anjie Wang,Baolian Yi,Yujiang Song
The scarcity and high cost of Pt-based electrocatalysts for the oxygen reduction reaction (ORR) hinder the practical application of proton exchange membrane fuel cells (PEMFCs). It is critical to replace platinum with non-noble metal electrocatalysts (NNMEs). Carbonized metalloporphyrins represent an important class of NNMEs, but most metalloporphyrins are costly and the corresponding NNMEs do not possess a high ORR activity. Herein, we report that the self-assembly of inexpensive hemin leads to porous nanomaterials in water under ambient conditions and subsequent heat-treatment of the unprecedented nanoporous hemin results in a magnetic NNME with a much enhanced ORR activity compared with directly carbonized hemin without self-assembly. The improvement of the ORR activity likely originates from the exposure of more ORR active sites, caused by the surface area increase of the nanoporous hemin after carbonization over that of micro-scale pristine hemin crystals. Moreover, the ORR activity of heat-treated nanoporous hemin is actually comparable to that of commercial Pt/C in alkaline solution. Additionally, the carbonized nanoporous hemin is much better than commercial Pt/C in terms of durability and tolerance to methanol. This study opens up a new avenue to the production of inexpensive metalloporphyrin-based NNMEs with a high ORR performance by using a self-assembly method in combination with traditional pyrolysis.
研究领域:
材料科学
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电化学
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能源材料
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PubMed
高影响因子
ChemCatChem
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2023
·Vol. 15
·期 23
·e202300883
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IF 4.5
Tianyu Zhang,Shensong Wang,Fengling Zhou,Sangaraju Shanmugam,Hasuck Kim,Xinyi Zhang
Graphical We report the synthesis of Co-doped Ni 3 C nanoparticles encapsulated in ultrathin carbon layers (CNCC) by in-situ thermal decomposition of organic-inorganic hybrid as high-performance HER electrocatalysts. With resurgent interest in green hydrogen as a key element in the transition to a renewable-energy economy, developing efficient, earth-abundant, and low-cost catalysts for hydrogen evolution reaction (HER) is becoming increasingly important but is still very challenging. Herein, we report the synthesis of Co-doped Ni 3 C nanoparticles encapsulated in ultrathin carbon layers (CNCC) by in-situ thermal decomposition of organic-inorganic hybrid as high-performance HER electrocatalysts. Experimental and density functional theory studies evidence that the substantial high-index (113) surfaces in synergy with a few atomic carbon layers contribute significantly to the activity and stability, while the electronic structure of Ni 3 C is optimized through tuning the Co content to enhance the intrinsic kinetics for HER. The CNCC exhibits excellent HER activities with overpotentials at 10 mA cm −2 (η 10 ) of 102 and 69 mV and Tafel slopes of 74 and 43 mV dec −1 in respective neutral and alkaline media along with a superior stability without noticeable decay up to 100 h. More importantly, the CNCC outperforms the benchmark Pt/C catalyst under high current density (>38 mA cm −2 ) in an alkaline electrolyte, showing great potential for practical hydrogen production.
研究领域:
材料科学
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电化学
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能源材料
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催化
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ACS Applied Materials & Interfaces
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2020
·
IF 8.758
Siyu Sheng,Bairu Shi,Cheng Wang,Liang Luo,Xiao Lin,Pengsong Li,Fanhong Chen,Zhicheng Shang,Hong Meng,Yun Kuang,Wen-Feng Lin,Xiaoming Sun
The bubbles electrochemically generated by gas evolution reactions are commonly driven off the electrode by buoyancy, a weak force used to overcome bubble adhesion barriers, leading to low gas-transporting efficiency. Herein, a Janus electrode with asymmetric wettability has been prepared by modifying two sides of a porous stainless-steel mesh electrode, with superhydrophobic polytetrafluoroethylene (PTFE) and Pt/C (or Ir/C) catalyst with well-balanced hydrophobicity, respectively, affording unidirectional transportation of as-formed gaseous hydrogen and oxygen from the catalyst side to the gas-collecting side during water splitting. “Bubble-free” electrolysis was realized while “floating” the Janus electrode on the electrolyte. Antibuoyancy through-mesh bubble transportation was observed while immersing the electrode with the PTFE side downward. The wettability gradient within the electrode endowed sticky states of bubbles on the catalyst side, resulting in efficient bubble-free gas transportation with 15-fold higher current density than submerged states.
研究领域:
电化学
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材料科学
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表面科学
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PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2016
·
IF 2.628
Tingting Zhang,Chuansheng He,Linbo Li,Yuqing Lin
The oxygen reduction reaction (ORR) is traditionally performed using noble-metals catalysts, e.g. Pt. However, these metal-based catalysts have the drawbacks of high costs, low selectivity, poor stabilities, and detrimental environmental effects. Here, we describe metal-free nitrogen-doped carbon nanoblocks (NCNBs) with high nitrogen contents (4.11%), which have good electrocatalytic properties for ORRs. This material was fabricated using a scalable, one-step process involving the pyrolysis of tris(hydroxymethyl)aminomethane (Tris) at 800 °C. Rotating ring disk electrode measurements show that the NCNBs give a high electrocatalytic performance and have good stability in ORRs. The onset potential of the catalyst for the ORR is −0.05 V (vs Ag/AgCl), the ORR reduction peak potential is −0.20 V (vs Ag/AgCl), and the electron transfer number is 3.4. The NCNBs showed pronounced electrocatalytic activity, improved long-term stability, and better tolerance of the methanol crossover effect compared with a commercial 20 wt% Pt/C catalyst. The composition and structure of, and nitrogen species in, the NCNBs were investigated using Fourier-transform infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and X-ray diffraction. The pyrolysis of Tris at high temperature increases the number of active nitrogen sites, especially pyridinic nitrogen, which creates a net positive charge on adjacent carbon atoms, and the high positive charge promotes oxygen adsorption and reduction. The results show that NCNBs prepared by pyrolysis of Tris as nitrogen and carbon sources are a promising ORR catalyst for fuel cells.
研究领域:
材料科学
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电化学
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纳米技术
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催化
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高影响因子
MATERIALS RESEARCH BULLETIN
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2026
·
IF 5.8
Huabo Li,Dong Bai,Lu Zhou
Eight post-synthesis acid treatments were systematically compared under identical polyol-derived Pt/C preparation conditions. • Citric acid treatment at pH 2 achieved 99% Pt loading efficiency and an ECSA of 106.2 m 2 gPt −1 . • The citric acid-treated catalyst delivered an ORR mass activity of 0.279 A mgPt −1 , exceeding that of commercial Pt/C. • After 30,000 potential cycles, the citric acid-treated catalyst showed a lower ECSA loss than commercial Pt/C (25.3% vs. 42.3%). Proton exchange membrane fuel cells (PEMFCs) are promising electrochemical energy-conversion devices, but their performance is limited by the sluggish kinetics of the oxygen reduction reaction (ORR). In this study, the effects of post-synthesis acid treatment on polyol-derived Pt/C catalysts supported on Vulcan XC-72 were systematically investigated. Eight chemically distinct acids, including citric, sulfuric, phosphoric, tartaric, oxalic, nitric, acetic, and hydrochloric acids, were compared under otherwise identical preparation conditions, followed by a separate citric-acid dosage series corresponding to final pH values of 2–5. The influences of acid chemistry and post-treatment pH on Pt retention, nanoparticle size and dispersion, Pt surface oxidation state, electrochemically active surface area (ECSA), ORR activity, and durability were evaluated. Thermogravimetric analysis showed that the citric-acid-treated catalyst exhibited a residual Pt fraction of 29.68 wt%, corresponding to approximately 99% of the nominal Pt loading. XRD and TEM analyses revealed Pt crystallite and particle sizes in the range of approximately 2.2–3.8 nm, with the citric-acid-treated catalyst showing relatively small and uniformly dispersed Pt nanoparticles. At pH 2, the citric-acid-treated catalyst achieved the highest ECSA of 106.2 m 2 gPt −1 and an ORR mass activity of 0.279 A mgPt −1 at 0.9 V vs. RHE, exceeding the values measured for commercial Johnson Matthey HiSPEC™ 3000 Pt/C (91.1 m 2 gPt −1 and 0.216 A mgPt −1 , respectively). XPS further showed that the citric-acid-treated catalyst retained a relatively high fraction of metallic Pt, consistent with its favorable electrochemical accessibility and surface state. After 30,000 potential cycles, the citric-acid-treated catalyst exhibited a lower ECSA loss than the commercial reference (25.3% vs. 42.3%) and less XRD-detectable crystallite coarsening. Single-cell measurements under matched cathode Pt loading also showed higher cell voltages for the citric-acid-treated catalyst over the investigated current-density range. These results indicate that post-synthesis citric acid treatment can improve Pt retention, nanoparticle dispersion, electrochemical accessibility, ORR activity, and structural durability through acid-dependent surface and Pt–carbon interfacial effects. The present protocol was demonstrated at a laboratory scale, yielding approximately 80 mg of catalyst per batch. Download: Download high-res image (152KB) Download: Download full-size image A comparative analysis was conducted on the oxygen reduction activity of Pt/C catalysts obtained under various chelating agents and their dosages. The optimal chelating agent and its corresponding amount were identified, and an in-depth investigation was carried out to understand the factors contributing to their superior performance.
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ACS Applied Energy Materials
·
2026
·
IF 5.5
Shenao Tian,Shang Li,Chongxue Zhao,Dong Xie,Mu Pan
Proton-exchange membrane fuel cells (PEMFCs) have emerged as a promising energy conversion technology due to their high energy efficiency, low operating temperature, zero pollutant emissions, and carbon neutrality, rendering them highly attractive for transportation and stationary power applications. However, enhancing the durability of Pt-based oxygen reduction reaction (ORR) catalysts while maintaining high activity remains a critical challenge for PEMFCs. In this study, a Pt/C@TPTZ450 ORR catalyst was synthesized via the surface modification of Pt/C with the nitrogen-containing organic small-molecule 2,4,6-tris(2-pyridyl)-1,3,5-triazine (TPTZ), resulting in the formation of an ultrathin nitrogen-containing coating layer (≈0.5 nm) that effectively stabilizes the catalyst structure. The modified catalyst exhibits enhanced ORR mass activity in rotating disk electrode (RDE) measurements compared with pristine Pt/C. More importantly, the TPTZ-derived coating effectively restricts the undesirable processes of Pt catalyst particle growth, carbon support corrosion, Pt migration, and Pt leaching during long-term operation. Consequently, the durability of the Pt/C@TPTZ450 catalyst is significantly improved compared to that of the pristine Pt/C catalyst. After 30,000 cycles of accelerated stress tests (ASTs), the membrane electrode assembly (MEA) with the Pt/C@TPTZ450 catalyst exhibits a voltage decay of only 22 mV at a current density of 0.8 A/cm2, accompanied by an electrochemical active surface area decay of 38.42%. These durability metrics fully meet the technical targets set by the U.S. Department of Energy (DOE) for proton-exchange membrane fuel cell catalysts. Furthermore, this work provides new insights and practical solutions for enhancing catalyst durability.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Lu Li,Jiahao Gu,Yaqi Ye,Jun Guo,Jie Zhao,Guifu Zou
Efficient and stable electrocatalysts are essential for generating continuous and clean hydrogen energy through electrochemical water splitting. Palladium (Pd) has been widely used in various catalytic reactions due to its unique electronic structures and chemical properties. Herein, we reported a facile synthesis strategy to homogeneously embed Pd nanoparticles in nitrogen-doped porous carbon fibers (Pd-PCNFs) through three successive processes of pre-oxidation, carbonization, and etching. The porous carbon fiber not only acts as a support matrix for highly dispersed Pd nanoparticles to avoid sintering in the high temperature process, but also provides efficient ion penetration and mass transport during the hydrogen evolution reaction (HER) process. More importantly, Raman and X-ray photoelectron spectroscopy (XPS) characterization confirmed the effective synergy between Pd nanoparticles and N-doped porous carbon fibers, which will help enhance the intrinsic electrocatalytic activity of Pd nanoparticles. Consequently, Pd-PCNFs-800 obtained by annealing at 800 °C exhibit significantly enhanced and stable electrocatalytic activity with an onset potential of 0 mV (0.5 M H 2 SO 4 ) and 40 mV (1 M KOH). It is noteworthy that the catalytic activity of Pd-PCNFs-800 is close to or better than commercial 10% Pd/C in different electrolytes. Impressively, in alkaline media, the activity of Pd-PCNFs-800 is even superior to commercial Pt/C at large current densities (>48.6 mA cm −2 ). This work provides a novel perspective to design and enrich the applications of Pd-based catalysts supported on carbon substrates.
研究领域:
材料科学
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电化学
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催化
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能源材料
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高影响因子
Nano Energy
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2023
·
IF 17.6
Rui Ma,Xun Cui,Xiaoxue Xu,Yonglin Wang,Gaoqiang Xiang,Likun Gao,Zhiqun Lin,Yingkui Yang
The rational design and facile synthesis of cost-effective and high-performance carbon-based catalysts for oxygen reduction reaction (ORR) is of great significance but remain challenging. Herein, we report the crafting of a robust Fe,N,P-codoped, ultrafine Fe 2 P nanocrystals decorated, highly hierarchical porous carbon nanoshells (denoted Fe,N,P-CNSs/Fe 2 P) via a simple yet robust one-step synergetic phosphorization and pyrolysis approach for highly-efficient ORR. Specifically, well-defined polypyrrole- co -polyaniline hollow nanospheres with a shell thickness of ≈ 43 nm (PPy- co -PANI-HNs) are first elaborately synthesized via a facile soft-templating (Triton X-100 micelles) copolymerization of pyrrole and aniline monomers . Subsequent one-step synergetic phosphorization and pyrolysis of PPy- co -PANI-HNs pre-impregnated with NaH 2 PO 2 ·H 2 O and FeCl 3 (H 2 PO 2 - ,Fe 3+ @PPy- co -PANI-HNs) yields Fe,N,P-CNSs/Fe 2 P with a well-crafted ultrathin nanoshell (shell thickness of ≈13 nm) architecture containing abundant hierarchical porosity . Remarkably, an alkaline electrolyte capitalizing on the resulting Fe,N,P-CNSs/Fe 2 P manifests excellent ORR performance with the half-wave and onset potentials ( E 1/2 of 0.854 V and E onset of 0.955 V) comparable to Pt/C, diffusion limited current density ( J L of −5.98 mA cm −2 ) higher than Pt/C, and long-time durability and methanol resistance better than Pt/C, demonstrating great potential as air cathode in zinc-air batteries (maximum power density of 170 mW cm −2 and specific capacity of 824.5 mA h g −1 ). Combined experimental and theoretical studies reveal that the impressive ORR performance of Fe,N,P-CNSs/Fe 2 P originates from simultaneous compositional (i.e., Fe,N,P-codoping and ultrafine Fe 2 P nanocrystals decorating) and structural (i.e., hierarchically porous ultrathin nanoshell architecture) tailoring enabled by the judicious one-step synergetic phosphorization and pyrolysis.
研究领域:
材料科学
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电化学
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纳米技术
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能源存储
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高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Zhiwen Xu,Guangyu Chen,Fei Yang,Juhee Jang,Guimei Liu,Fei Xiao,Yan Sun,Xiaoyi Qiu,Weiwei Chen,Dong Su,Meng Gu,Minhua Shao
The development of inexpensive and high-performance bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of crucial significance for rechargeable metal-air batteries , but remains challenging. Herein, we report an ingenious bifunctional oxygen electrocatalyst integrating ZIF-derived carbon-anchored Fe/Ni single atoms, FeNi alloy nanoparticles , and graphene support (denoted as Fe/Ni-NC||FeNi@G). Synergizing highly active Fe single atoms for the ORR and highly efficient FeNi alloy nanoparticles for the OER, the as-constructed Fe/Ni-NC||FeNi@G catalyst exhibits outstanding bifunctionality; the potential gap between the OER potential at 10 mA cm –2 and the ORR half-wave potential is only 0.618 V, outperforming the benchmark Pt/C + Ir/C catalyst and most transition metal-based bifunctional catalysts reported in the literature. More importantly, the Fe/Ni-NC||FeNi@G-driven zinc-air battery (ZAB) delivers a maximum power density of ∼200 mW cm –2 , a specific capacity of 876 mAh g –1 , and excellent cycling stability with negligible voltage decay up to 500 hours (3000 cycles). This work provides an effective approach to designing highly efficient non-noble metal multifunctional catalysts for practical applications in rechargeable metal-air batteries.
研究领域:
材料科学
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电化学
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能源存储
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催化
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2023
·
IF 19
Shoujie Guan,Jingxi Wang,Yang Yang,Xun Zhu,Jianping Zhou,Dingding Ye,Rong Chen,Hongwei Dai,Qiang Liao
With the emerging demand of implantable microelectronics, it essentially requires the fully integrated and reliable power supplies. The study reports a stretchable and flexible electrospinning-based glucose/O 2 biofuel cell with glucose oxidase bioanode, Pt/C cathode and thermoplastic polyurethane substrate, which is capable for adapting to the various stresses and strains caused by individual movement. The rigid benzene rings and elastic chain segments of thermoplastic polyurethane ensure its superior tensile property. Furthermore, the stable covalent connections between the activated carbon nanotubes (CNTs-COOH) and glucose oxidase inside 3D thermoplastic polyurethane network are established by amide reaction to ensure the rapid direct electron transfer of bioanode and stable power output of device in flexible environments. The biofuel cell exhibits an open circuit voltage of 0.575 V, and high-power density of 57 µW cm −2 in 5 mM glucose. Moreover, the power-generation properties of implantable biofuel cell keep steady, and its power density exhibits limited fluctuations on the dorsum of rat when bending, stretching, and twisting in 28 days. There is no obvious local inflammation or systemic abnormalities in rats. It satisfies the impressive biocompatible requirement, demonstrating the promising potential of electrospinning-based biofuel cell as a robust self-sustained power source for implantable electronics.
研究领域:
生物医学工程
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材料科学
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纳米技术
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生物化学
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高影响因子
危险品化学品经营许可证（带存储）