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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-11 · IF 15.7

Fine-tuning d-p hybridization in Ni-Bx cocatalyst for enhanced photocatalytic H2 production

Long Haoyu,Zhang Xidong,Zhang Zhenyi,Zhang Jianjun,Yu Jiaguo,Yu Huogen

The H 2 -evolution kinetics play a pivotal role in governing the photocatalytic hydrogen-evolution process. However, achieving precise regulation of the H-adsorption and H-desorption equilibrium (H ads /H des ) still remains a great challenge. Herein, we propose a fine-tuning d - p hybridization strategy to precisely optimize the H ads /H des kinetics in a Ni-B x modified CdS photocatalyst (Ni-B x /CdS). X-ray absorption fine-structure spectroscopy and theoretical calculations reveal that increasing B-atom amount in the Ni-B x cocatalyst gradually strengthens the d - p orbital interaction between Ni 3 d and B 2 p , resulting in a consecutive d -band broadening and controllable d -band center on Ni active sites. The above consecutive d -band optimization allows for precise modulation of the H ads /H des dynamics in the Ni-B x /CdS, ultimately demonstrating a remarkable H 2 -evolution activity of 13.4 mmol g -1 h -1 (AQE = 56.1 %). The femtosecond transient absorption spectroscopy further confirms the rapid electron-transfer dynamics in the Ni-B x /CdS photocatalyst. This work provides insights into the optimal design of prospective H 2 -evolution catalysts.

CAS / MDL: 74-94-2 1306-23-6
研究领域: 材料科学 · 催化化学
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Indium-nickel oxide nanocomposite for room temperature H2 gas detection and its sensing mechanism

Yuxiao Jiang,Kelin Hu,Jing Zhang,Yujuan Hu,Yuepeng Yang,Xihuan Yin,Peigen Huang

Lithium-ion batteries (LIBs) have a wide range of applications in energy storage power stations. However, thermal runaway of LIBs can lead to serious safety accidents and cause significant losses. Therefore, it is particularly important to carry out early security warning of LIBs. And H 2 is generated along with the growth of lithium dendrites , which can serve as an effective indicator for detecting LIBs before TR. In this paper, In 2 O 3 /NiO nanocomposites were prepared, and five groups of samples were systematically prepared by adjusting the molar ratio of In and Ni. X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and other test methods were used to characterize the prepared nanocomposites. Through experiments, the best samples among several groups of samples were determined. When the test gas is introduced, the resistance change of this optimal sensor is the greatest, indicating the best performance, which is significantly better than pure In 2 O 3 and pure NiO samples. Furthermore, compared to other gases, this nanocomposite sensor exhibits significant selectivity towards H 2 . The results show that In 2 O 3 /NiO is a promising candidate material for room temperature H 2 detection, and provide suggestions for the development of gas sensors with heterogeneous structures.

CAS / MDL: 207398-97-8 10101-97-0
研究领域: 材料科学 · 能源技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Hierarchical Ti3C2/BiVO4 microcapsules for enhanced solar-driven water evaporation and photocatalytic H2 evolution

Xin Xiong,Naila Arshad,Junyang Tao,Najah Alwadie,Gang Liu,Liangyou Lin,M.A.K Yousaf Shah,Muhammad Sultan Irshad,Jingwen Qian,Xianbao Wang

Desalination processes frequently require a lot of energy to generate freshwater and energy, which depletes resources. Their reliance on each other creates tension between these two vital resources. Herein, hierarchical MXene nanosheets and bismuth vanadate (Ti 3 C 2 /BiVO 4 )-derived microcapsules were synthesized for a photothermal-induced photoredox reaction for twofold applications, namely, solar-driven water evaporation and hydrogen (H 2 ) production. For this purpose, flexible aerogels were fabricated by introducing Ti 3 C 2 /BiVO 4 microcapsules in the polymeric network of natural rubber latex (NRL-Ti 3 C 2 /BiVO 4 ), and a high evaporation rate of 2.01 kg m −2 h −1 was achieved under 1-kW m −2 solar intensity. The excellent performance is attributed to the presence of Ti 3 C 2 /BiVO 4 microcapsules in the polymeric network, which provides balanced hydrophilicity and broadband sun absorption (96 %) and is aimed at plasmonic heating with microscale thermal confinement tailored by heat transfer simulations. Notably, localized plasmonic heating at the catalyst active sites of the Ti 3 C 2 /BiVO 4 heterostructure promotes enhanced photocatalytic H 2 production evolved after 4 h of reaction is 9.39 μmol, which is highly efficient than pure BiVO 4 and Ti 3 C 2 . This method turns the issue of water–fuel crisis into a collaborative connection, presenting avenues to collectively address the anticipated demand rather than fostering competition.

研究领域: 材料科学 · 环境科学 · 能源科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

High-purity H2 production from biomass through cascade processes based on alkaline thermal treatment

Xingyu Gong,Houfang Lu,Guojie Liu,Kejing Wu,Bin Liang

A cascade process consisting of three techniques of alkaline thermal treatment, catalytic steam reforming, and alkali absorption is introduced to produce high-purity H 2 . The effect of NaOH and biomass molar ratio is investigated for H 2 production, and the interactions between the three components was carried out specially to investigate the effect on H 2 and CH 4 production for the alkaline thermal treatment of real biomass. Synthesized mesoporous 10 wt% Ni/Al 2 O 3 catalyst is applied in steam reforming of CH 4 . The NaOH supported on CaO was used for the absorption of CO and CO 2 during the alkali absorption process. The results show that the high H 2 production of 68.04 mmol g −1 cellulose with a purity of 99.93 vol% is achieved under optimized conditions. The cascade process for sawdust results in a 103% increase in H 2 production compared with one-step alkaline thermal treatment, and the H 2 purity is greater than 99.9 vol%.

CAS / MDL: 9004-34-6 9014-63-5
研究领域: 能源与环境科学 · 化学工程
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Capacitance Catalysis: Positive and Negative Effects of Capacitance of Mo2C in Photocatalytic H2 Evolution

Li Luo,Dekang Li,Yuying Dang,Wei Wang,Guangsuo Yu,Jin Li,Baojun Ma

A non-noble metal cocatalyst with capacitance is cost-effective and has excellent photocatalytic H2 evolution performance for water splitting. But the intrinsic action of capacitance is unclear. Here, by controlling the capacitance of Mo2C, we reported a volcanic curve relationship between the photocatalytic activity of Mo2C/CdS and the capacitance of Mo2C. At the middle capacitance of 18.95 F/g of Mo2C-a4, Mo2C-a4/CdS exhibits the best H2 evolution activity of 5560 μmol/g/h. When Pt is introduced on the surface of Mo2C, the photocatalytic activity of (Pt/Mo2C-a4)/CdS is further enhanced to 8090 μmol/g/h. Comparing the activities between (Pt/Mo2C)/CdS and Mo2C/CdS with the capacitance of Mo2C, the activity ratio and difference values increase and finally reach a plateau with the increasing capacitance. Electrochemical and photoelectrochemical studies demonstrate that the capacitance of Mo2C has dual opposite effects (positive and negative) in photocatalytic reactions. The capacitance can capture electrons and store them, thereby enhancing the separation efficiency of photoexcited carriers of CdS. However, overlarge capacitance constrains the stored electrons and prevents them from releasing, thus decreasing the cocatalytic efficiency, which can be resolved in some degree by introducing some Pt on Mo2C. This work elucidates the dual effects of capacitance and puts forward the concept of capacitance catalysis.

研究领域: 材料科学 · 催化化学
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Journal of Materials Research and Technology-JMR&T · 2021 · IF 5.039

Behavior of synchronous reduction and nitridation of iron/vanadium oxides with NH3–H2 mixtures

Yongjie Liu,Ran Xin,Donglai Ma,Qingqing Hu,Yue Wang,Zhixiong You

Ferrovanadium nitride, which comprises V and N, is an important alloy additive for the production of high-strength low-alloy steel. As an efficient reducing agent and nitrogen source, ammonia gas is widely used in the preparation of metal nitrides. In this study, ferrovanadium nitride alloy powder is prepared by reducing and nitriding VO 2 /Fe 2 O 3 in NH 3 –H 2 gas mixtures with different nitriding potentials. Thermodynamic analysis indicate that the reduction and nitridation of VO 2 and Fe 2 O 3 is feasible. VO 2 is converted into VN, whereas Fe and Fe 4 N can be formed depend on the reaction conditions. Lower temperatures and higher nitriding potentials are beneficial to the formation of Fe 4 N. Based on Rietveld refinement analysis, the formation of Fe 4 N and the atomic occupancy of V and N in vanadium oxynitride, which is associated with the temperature, reaction time, and nitriding potential, is determined. A ferrovanadium nitride alloy powder with an O content of 0.26 wt.% is prepared by reducing and nitriding VO 2 /Fe 2 O 3 at 900 °C for 1 h at a nitriding potential of 4.4 × 10 −3  Pa −0.5 .

研究领域: 材料科学 · 冶金工程
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Flexible and lightweight Ti3C2Tx MXene@Pd colloidal nanoclusters paper film as novel H2 sensor

Zhengyou Zhu,Congcong Liu,Fengxing Jiang,Jing Liu,Xiumei Ma,Peng Liu,Jingkun Xu,Lei Wang,Rui Huang

Rational and smart design of hydrogen (H 2 ) sensors especially those featured with flexibility and light weight is highly desirable, to meet the requirements for future development of portable H 2 sensors. In this work, we demonstrate a novel paper film H 2 sensor employing Ti 3 C 2 T x MXene nanosheets with Pd colloidal nanoclusters (Pd CNC) as the activator. The MXene@ Pd CNC paper film was facilely prepared via an all-colloidal solution-based vacuum-filtration process, which is flexible, light-weight and endowed with a compact, glossy surface. The as-obtained MXene@ Pd CNC film sensor displayed moderate H 2 response at room temperature at either flat or bent states. Specially, the MXene@Pd CNC film sensor delivered a response time of (32 ± 7) s and a sensitivity of S = (23.0 ± 4.0)%@4% H 2 . In addition, the MXene@Pd CNC sensor enabled “in-situ-mode” H 2 detection directly along a piece of paper film with desired size. The strong H 2 adsorption into lattice of ultrafine Pd CNC altered the work function thus induced the electron doping of MXene, which explained the gas sensing mechanism. Therefore, the facilely designed MXene@Pd CNC sensor is believed to contribute to development of future portable and wearable sensing electronics.

研究领域: 材料科学 · 传感器技术 · 纳米科技
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Metal-free SiOC/g-C3N4 heterojunction composites with efficient visible-light photocatalytic H2 production

Jianmei Pan,Wei Shen,Yahai Zhang,Hua Tang,Haoyu Sun,Wenqiang Zhong,Xuehua Yan

Photocatalytic water splitting to product hydrogen (H 2 ) is a desired route to utilize solar energy into chemical energy. At present, most photocatalysts for H 2   generation contains metallic elements with high-cost, confined reserves, and environmentally   unfriendly. The exploitation of metal-free and efficient photocatalysts becomes   particularly   important. Herein, a new metal-free g-C 3 N 4 -based heterojunction composites were facilely produced via the ultrasonic assisted deposition and subsequent calcination from g-C 3 N 4 layers embedded with SiOC with prominent conductivity and large surface area. Systematic investigates suggested that the SiOC/g-C 3 N 4 heterojunctions exhibited eminently meliorated photocatalytic H 2 production efficiency. The optimum H 2 production rate (1020 μmol h −1 g −1 ) of the SiOC/g-C 3 N 4 photocatalyst is 3.2 and 25.5 folds that of g-C 3 N 4 and SiOC , respectively. The boosted photocatalytic activity primarily originates from the increased absorptivity of light, the markedly expedited charge migration and the impeded recombination of charge carriers. This study offers a new perspective for the scientific contrive and fabrication of high-quality heterojunction photocatalysts for solar energy utilization.

研究领域: 材料科学 · 能源科学
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ACTA PHYSICO-CHIMICA SINICA · 2023 · IF 10.9

Interfacial Engineering of Ultrathin 2D/2D NiPS3/C3N5 Heterojunctions for Boosting Photocatalytic H2 Evolution

Jiawei Hu,Kai Xia,Ao Yang,Zhihao Zhang,Wen Xiao,Chao Liu,Qinfang Zhang

This study focuses on exploring efficient photocatalysts for water splitting, which holds great potential for harnessing hydrogen (H 2 ) as a renewable energy source. Modulating the heterojunction interface is known to enhance charge carrier separation and solar energy utilization, thereby boosting photocatalytic activity. In this work, a mechanical mixing-assisted self-assembly approach was developed to construct a heterojunction between NiPS 3 (NPS) nanosheets (NSs) and C 3 N 5 (CN) NSs. Specifically, two-dimensional (2D) NPS NSs were tightly deposited on 2D CN NSs surface to gain a 2D/2D heterostructure. The photocatalytic performance of the synthesized photocatalysts was determined by their ability to generate H 2 through water splitting, both in deionized (DI) water and seawater, under visible light. The resulting NPS NSs/CN NSs (NPS/CN) composites possessed boosted photocatalytic hydrogen evolution (PHE) activity related to CN NSs and NPS NSs. This improvement was assigned to the synergistic effect of increased light-harvesting capacity and heterojunction formation. Nevertheless, an excessive amount of deposited NPS NSs on the surface of CN NSs was found to reduce the light absorption of the CN NSs component in the NPS/CN composites, resulting in decreased PHE activity. Therefore, it was determined that an appropriate mass ratio between the two components is necessary to achieve excellent photocatalytic activity for the NPS/CN composites. The optimized photocatalyst, referred to as 3-NPS/CN, demonstrated the highest visible-light-driven PHE efficiency of 47.71 μmol·h −1 , which was 2385.50 times higher than that of CN NSs. Moreover, 3-NPS/CN also exhibited excellent PHE activity in seawater, with a rate of 8.99 μmol·h −1 . The photoelectrochemical, steady-state photoluminescence (PL), time-resolved PL (TR-PL), steady-state surface photovoltage (SPV) and time-resolved surface photovoltage (TPV) techniques were performed to investigate the charge separation and migration behaviors of various photocatalysts. Based on the characterization results, our group proposed a reasonable PHE mechanism. In the NPS/CN photocatalysts, photo-induced electrons rapidly migrated from the conduction band (CB) of CN NSs to the CB of NPS NSs due to the potential difference and strong interfacial electronic coupling between the two materials. The photogenerated electrons accumulated on the CB of the NPS NSs component efficiently reduced protons to generate H 2 molecules. Concurrently, photogenerated holes on the valence band (VB) of CN NSs and NPS NSs were consumed with the assistance of triethanolamine (TEOA) molecules. This study presents a facile method for fabricating 2D/2D heterostructured photocatalysts, which hold promise for efficient and robust implementation in energy applications. Download: Download high-res image (82KB) Download: Download full-size image

研究领域: 材料科学 · 能源化学 · 光催化技术
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Chem Catalysis · 2026 · IF 10.7

Non-thermal H2 plasma regeneration of Au/MoS2 for CO2 oxidative dehydrogenation of propane

Yunshuo Wu,Xiaole Weng,Haiqiang Wang,Zhongbiao Wu

CO 2 -assisted oxidative dehydrogenation of propane (CO 2 -ODHP) is a promising route for propylene production and CO 2 utilization, but catalyst sintering under harsh reaction and coke-burning conditions limits industrial deployment. Here, we report a practical regeneration strategy in which non-thermal H 2 plasma rapidly restores Au/MoS 2 catalysts that were deactivated by sintering at 600°C. The plasma treatment regioselectively reconstructs supported Au nanoparticles into raft-like Au domains enriched in unsaturated Au δ+ sites and stabilized by strong Au−S interactions, and this effect results in a 6.3-fold increase in propylene yield. The regenerated catalyst shows industrially relevant propylene productivity, high operational stability, and repeated regenerability. Mechanistic studies indicate that the Au rafts, electronically promoted by subsurface sulfur, facilitate propane C−H activation while accelerating hydrogen spillover and propylene desorption. These findings establish plasma-driven catalyst reconstruction as an effective regeneration strategy for light-alkane dehydrogenation and sustainable olefin production.

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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Natural lignin as efficient catalyst for H2 production from NaBH4 methanolysis at low temperature

Miaolian Ma,Wanpeng Zhou,Yu Zhang,Qisen Huang,Zhixuan Hu,Liuzhang Ouyang

Herein, natural lignin is used for the first time as a catalyst for the methanolysis of NaBH 4 . Lignin exhibits excellent catalytic activity for the methanolysis of NaBH 4 , and the HGR value is as high as 20425 mL H 2 ·g cat −1 ·min −1 at room-temperature. It is still satisfactory even at − 20 ℃, with a HGR of 2182 mL H 2 ·g cat −1 ·min −1 , which is the highest value reported in the literature to date. In addition, the study of kinetic reaction orders for NaBH 4 methanolysis catalyzed by lignin indicates that the catalytic methanolysis of NaBH 4 obeys first-order kinetics with respect to both of NaBH 4 concentration and catalyst dosage. The activation energy for the methanolysis catalysis by lignin is calculated to be 19.5 kJ·mol −1 at low temperature of − 20 ∼ 25 ℃. The lignin retain over 66% of the original catalytic activity at the end of fifth consecutive reuse, and the catalytic activity can be completely recovered through simple acid treatment.

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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Incorporating graphene oxide into COF membranes enables ultrahigh proton conductivity and ultralow H2 crossover

Na Xing,Xiao Pang,Qingrui Meng,Zhong Gao,Leilang Zhang,Sijia Wang,Ziwen Liu,Yan Kong,Cuiting Ding,Hong Wu,Zhongyi Jiang

Proton exchange membranes (PEMs) are the core components of electrochemical hydrogen energy production, storage and conversion devices. It is a great challenge to develop PEMs with a combination of high proton conductivity, minimal H 2 crossover and mechanical robustness for achieving high efficiency and long-term stability in these devices. Here, a co-assembled PEM composed of ionic covalent organic framework (iCOF) nanosheets and functionalized graphene oxide (GO) nanosheets was presented. The iCOF (TpPa-SO 3 H) nanosheets and polydopamine-modified graphene oxide (DGO) nanosheets were co-assembled into TpPa-SO 3 H/DGO mixed nanosheets with ultrahigh aspect ratio, which were readily further processed into TpPa-SO 3 H/DGO co-assembled membranes. The abundant and uniformly distributed –SO 3 H groups on TpPa-SO 3 H nanosheets and the acid-base pairs formed between TpPa-SO 3 H and DGO nanosheets promoted proton conduction significantly. Additionally, the dense structured DGO nanosheets inhibited H 2 crossover remarkably, and the multiple interactions between TpPa-SO 3 H and DGO nanosheets enhanced mechanical strength . The resultant TpPa-SO 3 H/DGO co-assembled membrane exhibited an ultrahigh proton conductivity of 916.4 mS cm −1 (80 °C, 100% RH), an unprecedently low H 2 crossover of 9.7 barrer and a sufficient tensile stress of 87.8 MPa. The enhanced proton conduction and H 2 barrier property led to enhanced performance in both electrochemical hydrogen compression and single hydrogen fuel cells.

CAS / MDL: 124-07-2
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