Chinese Journal of Catalysis最新文献

Shielding active Fe oxide by surface oxide overlayers for harsh high-temperature water-gas shift reaction 通过表面氧化层屏蔽活性氧化铁，用于苛刻的高温水气转移反应

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64900-X

Rongtan Li, Xiangze Du, Xiaohui Feng, Jianyang Wang, Na Ta, Qiang Fu, Xinhe Bao

Oxide supports are well known to significantly influence the structure and properties of active oxide overlayers through strong oxide-support interactions. However, the effect of oxide overlayers on the underlying active oxide substrates remains poorly understood. Here, we report the controllable formation of ceria (CeO₂) overlayers on a hematite (Fe₂O₃) surface (CeO₂/Fe₂O₃) via a melting-wetting method. Submonolayer CeO₂ patches facilitate the partial reduction of surrounding Fe₂O₃ to active magnetite (Fe₃O₄) while effectively suppress further reduction of Fe₃O₄ to inactive metallic iron (Fe⁰) under harsh high-temperature water-gas shift (HT-WGS) conditions. We demonstrate this stabilization effect of surface oxide patches (MO_x, M = Ce, Cr, Mn, Mg, Al and Zn) on surrounding active Fe oxide sites via creating a shielding zone around each oxide patch. As a result, Fe₂O₃ catalysts covered with a small amount of CeO₂ surface overlayers (~1.8 wt%) exhibit remarkable stability at 450 °C for over 100 h, in contrast to rapid deactivation observed in pure Fe₂O₃ and industrial iron-chromium (6.5 wt% Cr) catalysts. Building on these findings, we have developed an advanced HT-WGS process that utilizes Cr-free catalysts and significantly reduces steam consumption. This study highlights the critical role of surface oxide overlayers in modulating the redox behavior and reactivity of underlying active oxide substrates, developing an interface confinement strategy for the design of robust and efficient oxide catalysts.

众所周知，氧化物载体通过强的氧化物-载体相互作用显著影响活性氧化物覆盖层的结构和性能。然而，氧化物覆盖层对底层活性氧化物衬底的影响仍然知之甚少。在这里，我们报道了通过熔融润湿法在赤铁矿（Fe2O3）表面（CeO2/Fe2O3）上可控地形成了铈（CeO2）覆盖层。亚单层CeO2斑块促进了周围Fe2O3部分还原为活性磁铁矿（Fe3O4），同时有效抑制了Fe3O4在恶劣的高温水气转换（HT-WGS）条件下进一步还原为活性金属铁（Fe0）。我们通过在每个氧化物斑块周围创建屏蔽区，证明了表面氧化物斑块（MOx, M = Ce, Cr, Mn, Mg， Al和Zn）对周围活性Fe氧化物位点的稳定作用。结果表明，表面覆盖少量CeO2 （~1.8 wt%）的Fe2O3催化剂在450°C下超过100小时表现出显著的稳定性，而纯Fe2O3和工业铁铬（6.5 wt% Cr）催化剂则表现出快速失活。基于这些发现，我们开发了一种先进的HT-WGS工艺，该工艺使用无铬催化剂，显著降低了蒸汽消耗。本研究强调了表面氧化物覆盖层在调节活性氧化物衬底的氧化还原行为和反应性方面的关键作用，为设计坚固高效的氧化物催化剂开发了一种界面约束策略。

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引用次数: 0

Interfacial Ni–N bond in g-C3N4/CoNi2S4 for enhanced photocatalytic CO2 conversion g-C3N4/CoNi2S4界面Ni-N键增强光催化CO2转化

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64923-0

Haonan Li , Wa Gao , Kangli Ma , Jian Lei , Olim Ruzimuradov , Akhtam Samiev , Ya Chen , Jingxiang Low , Yue Li

Cocatalyst loading has been extensively adopted in photocatalysis for enhancing photocatalytic performance. However, the sluggish interfacial charge dynamics between cocatalyst and photocatalyst has restricted the wide applications of such a strategy. Herein, we introduce the Ni–N interfacial bonds between lamellar nitrogen-vacancy-rich g-C₃N₄/CoNi₂S₄ nanoparticles (CN-V_N/CoNi₂S₄) composite material to bridge the photogenerated charge carrier separation at their interface. Specifically, extended X-ray absorption fine structure analysis reveals that these Ni–N interfacial bonds are originated from the bonding of CoNi₂S₄ with the nitrogen atoms adjacent to the nitrogen vacancies (V_N) in g-C₃N₄. Experimental evidence and theoretical calculations reveal that Ni–N interfacial bonds cannot only cause an intimate contact interface between CN-V_N/CoNi₂S₄, but also modulate the charge distribution on the CN-V_N and CoNi₂S₄, further boosting the photogenerated charge carrier separation. More interestingly, this tailored interfacial microenvironment significantly reduces the energy barrier for key intermediates formation while modulates the rate-determining step from *COOH generation to CO desorption, enabling efficient and controllable CO production. This work establishes a methodological framework for engineering advanced photocatalysts, enabling high-efficiency conversion of solar energy into clean fuels.

为了提高光催化性能，在光催化中广泛采用了载助催化剂。然而，助催化剂与光催化剂之间缓慢的界面电荷动力学限制了该策略的广泛应用。在此，我们在层状富氮空位的g-C3N4/CoNi2S4纳米颗粒（CN-VN/CoNi2S4）复合材料之间引入了Ni-N界面键，以在其界面处桥接光生载流子分离。具体来说，扩展的x射线吸收精细结构分析表明，这些Ni-N界面键是由CoNi2S4与g-C3N4中氮空位（VN）附近的氮原子成键形成的。实验证据和理论计算表明，Ni-N界面键不仅在CN-VN/CoNi2S4之间形成紧密接触界面，而且还可以调节CN-VN和CoNi2S4上的电荷分布，进一步促进光生载流子的分离。更有趣的是，这种定制的界面微环境显著降低了关键中间体形成的能量障碍，同时调节了从*COOH生成到CO解吸的速率决定步骤，实现了高效可控的CO生产。这项工作建立了一个工程先进光催化剂的方法框架，使太阳能高效转化为清洁燃料。

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引用次数: 0

Pure silica Beta zeolite supported Ag-Mn catalyst for efficient ozone decomposition 纯二氧化硅β沸石支持Ag-Mn催化剂高效臭氧分解

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(26)64956-X

Feng Li , Ye Ma , Mingyu Wan , Yating Lv , Jiamin Yuan , Shichao Han , Houyu Ma , Liang Wang , Xiangju Meng , Anmin Zheng , Yanhang Ma , Feng-Shou Xiao

Catalytic decomposition of ozone is considered as one of the most effective, economically viable, and promising strategies for ozone abatement. In a number of oxide-supported Ag catalysts, manganese oxide-based catalysts have been identified with superior activities, but there are still challenges for Ag sintering and competitive adsorption of water under humid conditions, which strongly hinder their catalytic performances. Herein, we prepared a pure silica Beta zeolite supported Ag-Mn catalysts (Ag-Mn/Beta-Si), exhibiting excellent catalytic properties in the decomposition of ozone, which is reasonably attributed to the in-situ formed AgMnO₂ on the pure silica Beta zeolite, where the formed AgMnO₂ as a new active site prevents the sintering of Ag NPs and the hydrophobicity of the pure silica Beta zeolite is favorable for hindering water adsorption on the active sites under humid conditions. These hypotheses have been evidenced by theoretical simulations of the mean square displacement and diffusion coefficient of water molecules and experimental results of sample transmission electron microscopy images.

臭氧的催化分解被认为是最有效的、经济上可行的和有前途的臭氧减排策略之一。在许多氧化物负载的银催化剂中，氧化锰基催化剂已被认为具有优越的活性，但在潮湿条件下银的烧结和水的竞争性吸附仍然存在挑战，这严重阻碍了它们的催化性能。本文制备了一种纯二氧化硅β沸石负载的Ag- mn催化剂（Ag- mn / β -si），在臭氧分解中表现出优异的催化性能，这合理地归因于纯二氧化硅β沸石上原位形成的AgMnO2，其中形成的AgMnO2作为新的活性位点阻止了Ag NPs的烧结，纯二氧化硅β沸石的疏水性有利于阻碍潮湿条件下活性位点上的水吸附。水分子的均方位移和扩散系数的理论模拟以及样品透射电镜图像的实验结果证明了这些假设。

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引用次数: 0

Coupling silver dual atoms and nanoparticles on carbon support for efficient electroreduction N2 to ammonia 偶联银双原子和纳米颗粒在碳载体上的高效电还原N2到氨

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64910-2

Chang Liu , Mei Wang , Xiangming Liang , Tongbu Lu

Electrocatalytic N₂ reduction reaction (eNRR) is a green and sustainable approach for producing ammonia. Herein, we synthesized a Ag_2-Ag_NPs@C catalyst by coupling dual-atom Ag sites (Ag₂) and Ag nanoparticle (Ag_NPs) on the carbon support, which exhibits excellent eNRR performance, with a high NH₃ yield rate of 139.9 μg h^–1 mg^–1_cat. and an outstanding Faradaic Efficiency of 74.2%, which are superior to those of most reported eNRR catalysts. Density functional thoery calculations and in-situ infrared spectroscopy analysis demonstrate that in Ag₂-Ag_NPs@C catalyst, Ag_NPs facilitate water dissociation to produce H* intermediate that supplies to adsorbed *N₂ on the Ag₂ site for promoting the formation of *NNH key intermediate, thus lowering the Gibbs free energy of rate-determining step and substantially enhancing the eNRR performance. This work opens up new avenues for developing efficient electrocatalytic nitrogen reduction catalysts via synergistic effect.

电催化N2还原反应（eNRR）是一种绿色、可持续的合成氨方法。本文通过在碳载体上偶联双原子银位（Ag2）和银纳米粒子（AgNPs）合成了一种Ag2-AgNPs@C催化剂，该催化剂具有优异的eNRR性能，NH3产率高达139.9 μg h-1 mg-1cat。Faradaic效率为74.2%，优于大多数已报道的eNRR催化剂。密度泛函理论计算和现场红外光谱分析表明，在Ag2-AgNPs@C催化剂中，AgNPs促进水解离生成H*中间体，提供给Ag2位点上吸附的*N2，促进*NNH关键中间体的形成，从而降低了速率决定步骤的吉布斯自由能，大大提高了eNRR性能。本研究为利用协同效应开发高效的电催化氮还原催化剂开辟了新的途径。

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引用次数: 0

Synergistic electrode-electrolyte coupling enabled highly efficient and durable high entropy intermetallic-based electrocatalyst for oxygen reduction reaction 电极-电解质的协同耦合使得氧还原反应中高效、耐用的高熵金属间基电催化剂成为可能

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64873-X

Weiping Xiao, Yue Zhang, Na Wang, Xiaofei Yang

Developing highly efficient and robust Pt-based electrocatalysts for oxygen reduction reaction (ORR) remains a substantial challenge due to the sluggish kinetics of proton-coupled electron transfer (PCET) process. Herein, an effective innovation strategy involves the rational construction of supported high-entropy intermetallics (HEIs) Pt₄FeCoNiSn, and its coupling with the ionic liquid [MTBD]⁺ is developed to simultaneously facilitate PCET steps of ORR. The anchoring effect of the substrate Co-NC and the induction effect of Sn atom conspicuously promote the formation of ordered Pt₄FeCoNiSn intermetallics at lower temperature. The multiple electron effects of HEIs and strong metal-support interactions enable Pt₄FeCoNiSn/CoNC with the half-wave potential (E_1/2) of 0.906 V in 0.1 mol L^–1 HClO₄ solution and 0.958 V in 0.1 mol L^–1 KOH solution, and long-term stability over 70 K cycles. Further [MTBD]⁺ modification of electrocatalyst leads to the enhancement in ORR performance, where the [MTBD]⁺ promotes the accumulation of reaction intermediates and increases the proportion of weakly hydrogen-bonded water at the electrode-electrolyte interface, thereby accelerating proton transfer rate during the ORR process. The Zn-air battery assembled by Pt₄FeCoNiSn/CoNC as oxygen electrode exhibits a high maximal power density of 190.2 mW cm^–2 at current density of 279.4 mA cm^–2, superior to those of Pt/C.

由于质子耦合电子转移（PCET）过程动力学缓慢，开发高效、稳健的氧还原反应（ORR）电催化剂仍然是一个巨大的挑战。本文提出了一种有效的创新策略，即合理构建支撑型高熵金属间化合物（HEIs） Pt4FeCoNiSn，并将其与离子液体[MTBD]+耦合，同时促进ORR的PCET步骤。在较低温度下，衬底Co-NC的锚定效应和Sn原子的诱导效应显著地促进了有序Pt4FeCoNiSn金属间化合物的形成。HEIs的多重电子效应和强金属-载体相互作用使Pt4FeCoNiSn/CoNC在0.1 mol L-1 HClO4溶液和0.1 mol L-1 KOH溶液中的半波电位（E1/2）分别为0.906 V和0.958 V，且在70 K循环内长期稳定。进一步对电催化剂进行[MTBD]+改性可以提高ORR性能，其中[MTBD]+促进了反应中间体的积累，增加了电极-电解质界面处弱氢键水的比例，从而加快了ORR过程中质子的转移速率。以Pt4FeCoNiSn/CoNC为氧电极组装的锌空气电池在电流密度为279.4 mA cm-2时，最大功率密度为190.2 mW cm-2，优于Pt/C。

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引用次数: 0

An active and durable anode catalytic layer with in-situ exsolved Pd-Ni nanoparticles for protonic ceramic fuel cells on hydrocarbon fuels 一种用于碳氢燃料质子陶瓷燃料电池的活性和耐用的原位溶解Pd-Ni纳米阳极催化层

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64913-8

Wenjie Gong, Yangsen Xu, Hao Liu, Wanbin Lin, Zhiwei Du, Yixuan Huang, Jiang Liu, Yu Chen

Operating hydrocarbons on protonic ceramic fuel cells (PCFCs) is promising and attractive, on account of their high energy conversion efficiency and potential for low carbon emissions compared to traditional thermal power generation. However, poor coking tolerance and insufficient catalytic activity at intermediate temperatures greatly hinder the development of PCFCs on hydrocarbons. Exploring a catalytic layer with high activity and durability is an effective way to achieve high-performance PCFCs on hydrocarbon fuels. Herein, we report an anode catalytic layer (ACL) with an optimized formula of Pd_0.01Ni_0.09Ce_1.9O_2–δ (P1NC). Pd-Ni alloy nanoparticles are exsolved from the ACL under a hydrogen atmosphere. The high oxygen vacancy concentration in P1NC has shown a positive effect on the oxygen storage capacity, which may facilitate carbon gasification, thereby reducing performance degradation during PCFC operation, as supported by the Raman and scanning electron microscopy observations. PCFCs with this ACL achieved a decent peak power density (P_max) of 1.20 W cm^–2 and stably operated at 0.2 A cm^–2 at 650 °C on CH₄. In addition, the cells with P1NC ACL exhibited encouraging P_max of 1.00 and 0.87 W cm^–2 at 650 °C on liquid fuels such as methanol and ethanol, respectively, exhibiting good fuel flexibility.

与传统的火力发电相比，质子陶瓷燃料电池（pcfc）具有高能量转换效率和低碳排放的潜力，因此在质子陶瓷燃料电池（pcfc）上运行碳氢化合物是很有前途和吸引力的。然而，较差的焦化耐受性和中温催化活性不足极大地阻碍了pcfc在烃类上的发展。探索具有高活性和耐久性的催化层是在烃类燃料上实现高性能pcfc的有效途径。本文报道了一种优化配方为pd0.01 ni0.09 ce1.90 o2 -δ (P1NC)的阳极催化层（ACL）。Pd-Ni合金纳米颗粒在氢气气氛下从ACL中析出。拉曼和扫描电镜观察结果表明，P1NC中高氧空位浓度对氧储存能力有积极影响，这可能有助于碳气化，从而减少PCFC运行过程中的性能下降。具有该ACL的pcfc实现了1.20 W cm-2的峰值功率密度（Pmax），并且在650°C的CH4中稳定地工作在0.2 a cm-2。此外，具有P1NC ACL的电池在650°C液体燃料（如甲醇和乙醇）上的Pmax分别为1.00和0.87 W cm-2，表现出良好的燃料柔韧性。

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引用次数: 0

Citric directional coordination for efficient photocatalytic synthesis of H2O2 with high value-added β-Ketoglutaric acid 柠檬酸定向配位用于高附加值β-酮戊二酸高效光催化合成H2O2

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64885-6

Jing Zhang , Xidong Zhang , Kaiyan Wang , Xuefei Wang , Ping Wang , Feng Chen , Huogen Yu

Photocatalytic hydrogen peroxide (H₂O₂) production offers a green alternative to the traditional anthraquinone process but remains limited by inefficient charge separation and underutilized photogenerated holes. Herein, we present a spatially resolved coordination strategy to couple efficient H₂O₂ generation with selective oxidation of biomass-derived hydroxy acids. Anisotropic Au-modified BiVO₄ photocatalysts were constructed, where Au nanoparticles on the (010) facet promoted H₂O₂ formation, while undercoordinated Bi atoms on the (110) facet selectively oxidized citric acid (CA). A five-membered chelate ring formed between β-hydroxyl and carboxyl groups of CA and surface Bi atoms, enabling directional coordination that enhanced hole extraction and guided a selective decarboxylation pathway to produce acetone dicarboxylic acid with 99% selectivity. This dual-functional design achieved a high H₂O₂ production rate (~0.6 mmol L^–1 h^–1) and exhibited broad applicability to other hydroxy acids. This work provides mechanistic insights into photocatalyst-substrate interactions and establishes a generalizable strategy for integrating H₂O₂ photosynthesis with value-added chemical production under solar irradiation.

光催化过氧化氢（H2O2）生产为传统的蒽醌工艺提供了一种绿色替代方案，但仍然受到低效率的电荷分离和未充分利用的光生孔的限制。在此，我们提出了一种空间解决的协调策略，将有效的H2O2生成与生物质衍生的羟基酸的选择性氧化结合起来。构建了各向异性Au修饰的BiVO4光催化剂，其中（010）面的Au纳米粒子促进H2O2的形成，而（110）面的欠配位Bi原子选择性氧化柠檬酸（CA）。在CA的β-羟基和羧基与表面Bi原子之间形成了一个五元螯合环，实现了定向配位，增强了空穴的提取，并引导了选择性脱羧途径，以99%的选择性生产丙酮二羧酸。这种双功能设计实现了较高的H2O2产率（~0.6 mmol L-1 h-1），并且对其他羟基酸具有广泛的适用性。这项工作提供了光催化剂-底物相互作用的机理见解，并建立了在太阳照射下将H2O2光合作用与增值化学生产相结合的通用策略。

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引用次数: 0

Alleviating hydroxyl poisoning on Ru through competitive adsorption regulation using anatase-rutile TiO2 heterostructures in alkaline hydrogen oxidation reaction 锐钛矿-金红石型TiO2异质结构在碱性氢氧化反应中竞争性吸附调控对Ru的羟基中毒

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64853-4

Jie Gao , Jing Liu , Mengdi Wang , Nuo Sun , Hao Hu , Xuejing Cui , Xin Zhou , Luhua Jiang

Ruthenium (Ru) is a promising electrocatalyst for the alkaline hydrogen oxidation reaction (HOR), yet it suffers from deactivation at higher potentials due to excessive oxophilicity, which leads to hydroxyl adsorption poisoning. Here, we report a tri-phase heterostructured catalyst (Ru-P25-TiO₂) comprising Ru with anatase (A-) and rutile (R-)TiO₂. This catalyst exhibits remarkable HOR activity, delivering 0.82 mA μg_Ru^‒1 along with superior electrochemical stability up to 0.9 V vs. RHE, positioning it as the state-of-the-art electrocatalyst for HOR. This enhanced performance is attributed to the optimized electron distribution and a tailored d band structure at the Ru surface, enabled by strong metal and support interaction, which weakens both hydrogen binding energy and hydroxyl binding energy. The highly oxyphilic P25-TiO₂ facilitates hydroxyl adsorption and establishes a continuous hydrogen-bond network at the catalyst/electrolyte interface, thereby promoting OH⁻ transport and alleviating competitive OH adsorption on the Ru surface. The synergistic interplay between anatase and rutile TiO₂ ideally endows Ru with both superior activity and excellent electrochemical stability. This work not only unravels the intrinsic role of biphasic TiO₂ in tailoring Ru electrocatalysis but also provides a generalizable synergistic heterostructure design strategy for developing efficient and durable electrocatalysts.

钌（Ru）是一种很有前途的碱性氢氧化反应（HOR）电催化剂，但由于其亲氧性太强，在高电位下会失活，从而导致羟基吸附中毒。本文报道了一种由Ru、锐钛矿（a -）和金红石（R-）TiO2组成的三相异质结构催化剂（Ru- p25 -TiO2）。与RHE相比，该催化剂具有出色的HOR活性，可提供0.82 mA μgRu-1以及高达0.9 V的优异电化学稳定性，使其成为最先进的HOR电催化剂。这种增强的性能归因于Ru表面优化的电子分布和定制的d带结构，通过强金属和载体的相互作用，减弱了氢结合能和羟基结合能。P25-TiO2具有高度亲氧性，有利于羟基的吸附，并在催化剂/电解质界面建立连续的氢键网络，从而促进OH的⁻传输，减轻OH在Ru表面的竞争性吸附。锐钛矿与金红石型TiO2之间的协同作用使Ru具有优异的活性和优异的电化学稳定性。这项工作不仅揭示了双相TiO2在定制Ru电催化中的内在作用，而且为开发高效耐用的电催化剂提供了一种可推广的协同异质结构设计策略。

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引用次数: 0

Sacrificial conversion of metal sulfide precursors into active oxyhydroxide catalysts for enhanced oxygen evolution reaction 牺牲金属硫化物前驱体转化为活性氢氧催化剂以增强析氧反应

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64876-5

Xinran Sun , Mengtian Huo , Jianhang Sun , Yu Liang , Kaichi Qin , Haoyang Zhang , Zihao Xing , Jinfa Chang

Transition metal sulfides (TMSs) are promising electrocatalysts for the oxygen evolution reaction (OER) due to their tunable spin states, diverse metal-sulfur coordination environments, and controllable electronic structures. However, their structural instability under anodic conditions remains a critical challenge. In particular, the mechanisms governing active-phase formation and the identification of true catalytically active sites during surface reconstruction require further investigation. Herein, we report a cubic, self-assembled FeCoS₂/FeS₂ heterostructure catalysts. Through sulfur doping and electrochemical activation-induced surface reconstruction, the catalyst achieves 10 mA cm⁻² current density at an overpotential of only 287 mV in 1.0 mol L⁻¹ KOH after 1000 cycles. Experimental and in-situ spectroscopy analyses reveal that the heterogeneous interface enhances electron transfer, while dynamic reconstruction generates a highly active metal (oxy)hydroxide phase as the primary catalytically active species. This work provides mechanistic insights into the surface reconstruction of TMSs, and offers a viable strategy for designing efficient and durable non-noble metal electrocatalysts.

过渡金属硫化物（tms）具有自旋态可调、金属硫配位环境多样、电子结构可控等特点，是很有前途的析氧反应电催化剂。然而，它们在阳极条件下的结构不稳定性仍然是一个关键的挑战。特别是，控制活性相形成的机制和表面重建过程中真正催化活性位点的识别需要进一步研究。本文报道了一种立方的、自组装的FeCoS2/FeS2异质结构催化剂。通过硫掺杂和电化学活化诱导的表面重构，在1.0 mol L−1 KOH条件下，经过1000次循环，催化剂的过电位仅为287 mV，电流密度为10 mA cm−2。实验和原位光谱分析表明，非均相界面增强了电子转移，而动态重构产生了高活性的金属（氧）氢氧化物相作为主要催化活性物质。这项工作为tms的表面重建提供了机理见解，并为设计高效耐用的非贵金属电催化剂提供了可行的策略。

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引用次数: 0

Ruthenium-tungsten alloy nanoparticles accelerate the cascade hydrogenation-ring opening of furfurals to linear ketones 钌钨合金纳米颗粒加速糠醛级联加氢环开环成线性酮

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/S1872-2067(25)64911-4

Peng Huang , Zhijun Xie , Yong Guo , Jun Wang , Ji-Jun Zou , Qiang Deng

The metal-acid bifunctional catalyzed conversion of furfurals to linear ketones is crucial but challenging for sustainable chemical synthesis owing to the tendency for over hydrogenation and overacid-catalyzed reaction pathways over traditional catalysts. Herein, ruthenium-tungsten (RuW) alloy nanoparticle-supported catalysts (such as, RuW/SiO₂, RuW/Al₂O₃, RuW/C) were prepared via incipient wetness impregnation followed by H₂ reduction, showing a cascade hydrogenation-ring opening transformation of furfural to 5-hydroxy-2-pentanone with an unprecedented yield of 86.2% at a mild temperature of 80 °C. Catalytic mechanism studies confirmed that hydrogen spillover from RuW alloy sites to WO_x sites generated H⁺-H^‒ pairs in situ, which functioned as atypical active sites for the furfural hydrogenation step and offered Brönsted acidic sites for the ring opening of furan alcohol, thereby facilitating the facile preparation of 5-hydroxy-2-pentanone. Furthermore, the catalyst exhibited broad applicability for synthesizing linear ketones from various furfurals (i.e., 5-methyl furfural and 5-hydroxymethyl furfural). This study demonstrated interesting bifunctional catalysis through harnessing hydrogen spillover to form transient H⁺-H^‒ pairs, enabling a challenging cascade reaction pathway toward an efficient linear ketone synthesis.

金属-酸双功能催化糠醛转化为线性酮是至关重要的，但由于与传统催化剂相比有过氢化和过酸催化反应途径的趋势，因此对可持续化学合成具有挑战性。本文采用湿浸渍法制备钌钨（RuW）合金纳米颗粒负载催化剂（如RuW/SiO2、RuW/Al2O3、RuW/C），再进行H2还原，在80℃的温和温度下，糠醛通过级联加氢开环转化为5-羟基-2-戊酮，收率达到了86.2%。催化机理研究证实，氢从RuW合金位点溢出到WOx位点，原位生成H+-H -对，作为糠醛加氢步骤的非典型活性位点，为呋喃醇开环提供Brönsted酸性位点，便于制备5-羟基-2-戊酮。此外，该催化剂对各种糠醛（即5-甲基糠醛和5-羟甲基糠醛）合成线性酮具有广泛的适用性。本研究通过利用氢溢出形成瞬态H+-H -对，展示了有趣的双功能催化作用，为高效的线性酮合成提供了具有挑战性的级联反应途径。

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引用次数: 0