Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60471-8

Yang LI , Bowen WU , Zhipeng YU , He YANG , Lijun JIN , Haoquan HU

Experimental studies on co-pyrolysis of coal and lignin are carried out on a fixed-bed reactor to investigate composition and transformation of the co-pyrolysis products. The results show that co-pyrolysis reduces yield of char and promotes yield of gas, the maximum pyrolysis gas yield increases by 33.1%. Co-pyrolysis has a significant promotion effect on generation of CH₄ and CO. The interaction between the pyrolyzed volatile fractions of coal and lignin shows the most pronounced interaction at a coal to lignin mixing ratio of 1:1, and the pyrolysis tar yield shows a positive synergistic effect. Guaiacols are converted to monophenols and bisphenols during the co-pyrolysis process. Content of monophenols and bisphenols increase by 2.9% and 9.8%, respectively, while content of guaiacols decreases by 5.1% compared with the theoretically calculated values. The breakage of carbonyl and carboxyl groups, and the interaction with volatile components are enhanced, which inhibits formation of ethers, aldehydes and acids, and promotes generation of phenols, release of oxygenated gases and stabilization of pyrolysis tar. The introduction of lignin into coal pyrolysis also significantly promotes the upgrading of tar in which light components is nearly 90%.

在固定床反应器上对煤和木质素的共热解进行了实验研究，以探讨共热解产物的组成和转化。结果表明，共热解降低了炭的产率，提高了气的产率，最大热解气产率提高了 33.1%。共热解对生成 CH4 和 CO 有显著的促进作用。煤与木质素的混合比为 1:1 时，煤的热解挥发分与木质素之间的相互作用最为明显，热解焦油产率显示出积极的协同效应。愈创木酚在共热解过程中转化为单酚和双酚。与理论计算值相比，单酚和双酚的含量分别增加了 2.9% 和 9.8%，而愈创木酚的含量则减少了 5.1%。羰基和羧基的断裂以及与挥发性成分的相互作用增强，从而抑制了醚、醛和酸的形成，促进了酚的生成、含氧气体的释放和热解焦油的稳定。在煤热解过程中引入木质素还能显著促进焦油的升级，其中轻组分占近 90%。

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引用次数: 0

Enhancing photo-generated carriers transfer of K-C3N4/UiO-66-NH2 with Er doping for efficient photocatalytic oxidation of furfural to furoic acid 掺杂 Er 增强 K-C3N4/UiO-66-NH2 的光生载流子转移，实现糠醛到糠酸的高效光催化氧化

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60469-X

Haocun WANG, Lingtao LIU, Junjie BIAN, Chunhu LI

Biomass-derived platform molecules, such as furfural, are abundant and renewable feedstock for valuable chemical production. It is critical to synthesize highly efficient photocatalysts for selective oxidation under visible light. The Er@K-C₃N₄/UiO-66-NH₂ catalyst was synthesized using a straight-forward hydrothermal technique, and exhibited exceptional efficiency in the photocatalytic oxidation of furfural to furoic acid. The catalyst was thoroughly characterized, confirming the effective adjustment of the band gap energy of Er@K-C₃N₄/UiO-66-NH₂. Upon the optimized reaction conditions, the conversion rate of furfural reached 89.3%, with a corresponding yield of furoic acid at 79.8%. The primary reactive oxygen species was identified as ·O− 2 from ESR spectra and scavenger tests. The incorporation of Er and K into the catalyst enhanced the photogenerated carriers transfer rate, hence increasing the separating efficiency of photogenerated electron-hole pairs. This study expands the potential applications of rare earth element doped g-C₃N₄ in the photocatalytic selective oxidation of furfurans.

从生物质中提取的平台分子（如糠醛）是一种丰富的可再生原料，可用于生产有价值的化学产品。合成在可见光下进行选择性氧化的高效光催化剂至关重要。Er@K-C3N4/UiO-66-NH2 催化剂采用简单的水热技术合成，在光催化氧化糠醛为糠酸的过程中表现出卓越的效率。对催化剂进行了全面表征，证实了 Er@K-C3N4/UiO-66-NH2 带隙能的有效调节。在优化的反应条件下，糠醛的转化率达到 89.3%，相应的糠酸收率为 79.8%。根据 ESR 光谱和清除剂测试，确定主要活性氧为 -O- 2。催化剂中加入 Er 和 K 可提高光生载流子的转移率，从而提高光生电子-空穴对的分离效率。这项研究拓展了掺杂稀土元素的 g-C3N4 在光催化选择性氧化呋喃中的潜在应用。

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引用次数: 0

Controllable synthesis of CuAlO2 via solid-phase method and its catalytic performance for methanol steam reforming to hydrogen 固相法可控合成 CuAlO2 及其在甲醇蒸汽转化制氢过程中的催化性能

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60473-1

Shaojun QING , Xun SUN , Xinglong LI , Lei WANG , Zhiwei WU , Jianguo WANG

This study explores the controllable synthesis of CuAlO₂ using copper hydroxide and pseudo-boehmite powders as raw materials via a simple solid-phase ball milling method, along with its catalytic performance investigation in methanol steam reforming (MSR). Various catalysts were prepared under different conditions, such as calcination temperature, calcination atmosphere, and heating rate. Characterization techniques including BET, XRD, XPS, SEM and H₂-TPR were employed to analyze the samples. The results revealed significant effects of calcination temperature on the phase compositions, specific surface area, reduction performance, and surface properties of the CA-T catalysts. Based on the findings, a synthesis route of CuAlO₂ via the solid-phase method was proposed, highlighting the importance of high calcination temperature, nitrogen atmosphere, and low heating rate for CuAlO₂ formation. Catalytic evaluation data demonstrated that CuAlO₂ could catalyze MSR without pre-reduction, with the catalytic performance of CA-T catalysts being notably influenced by calcination temperature. Among the prepared catalysts, the CA-1100 catalyst exhibited the highest catalytic activity and stability. The findings of this study might be useful for the further study of the catalytic material for sustained release catalysis, including the synthesis of catalytic materials and the regulation of sustained release catalytic performance.

本研究探讨了以氢氧化铜和假沸石粉末为原料，通过简单的固相球磨法可控合成 CuAlO2，并研究了其在甲醇蒸汽转化（MSR）中的催化性能。在煅烧温度、煅烧气氛和加热速率等不同条件下制备了各种催化剂。采用 BET、XRD、XPS、SEM 和 H2-TPR 等表征技术对样品进行了分析。结果表明，煅烧温度对 CA-T 催化剂的相组成、比表面积、还原性能和表面特性有显著影响。根据研究结果，提出了固相法合成 CuAlO2 的路线，强调了高煅烧温度、氮气氛和低加热速率对 CuAlO2 形成的重要性。催化评估数据表明，CuAlO2 无需预还原即可催化 MSR，CA-T 催化剂的催化性能受煅烧温度的影响明显。在制备的催化剂中，CA-1100 催化剂的催化活性和稳定性最高。本研究的结果可能有助于进一步研究用于缓释催化的催化材料，包括催化材料的合成和缓释催化性能的调控。

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引用次数: 0

Architecture of core-shell Ce-OMS-2@CeO2 catalyst and its SCR activity and SO2+H2O tolerance performance at low-temperature 核壳 Ce-OMS-2@CeO2 催化剂的结构及其低温 SCR 活性和 SO2+H2O 耐受性能

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60465-2

Geyu DAI, Yuewang PENG, Chao YU, Bihong LÜ, Xiaomin WU, Guohua JING

It is a challenge to develop highly sulfur dioxide and water (SO₂+H₂O) resistance for the low-temperature selective catalytic reduction (SCR) catalysts of nitrogen oxide (NO_x) in the non-electric-power industry. In this paper, core-shell and loaded type of Ce-OMS-2 complexes (Ce-OMS-2@CeO₂ and CeO₂/Ce-OMS-2) were successfully prepared. Their textural properties were characterized and catalytic performance were carried out. The results showed that the core-shell Ce-OMS-2@CeO₂ material could maintain the mesoporous structure and significantly improve the mass transfer and adsorption of the reaction gas NO, thus improving the SCR efficiency. On the contrary, for the loaded CeO₂/Ce-OMS-2 catalyst, large amounts of CeO₂ deposited on the surface of Ce-OMS-2 and blocked the mesoporous structure. Furthermore, SO₂ reacted with CeO₂/Ce-OMS-2 to form lots of metal sulfate (manganese sulfate or cerium sulfate), which led to the deactivation of the active Mn sites. Therefore, the CeO₂/Ce-OMS-2 catalyst exhibited the low SCR activity and poor SO₂+H₂O tolerance during the SCR reaction. We also clarify the reason for the anti-sulfur of core-shell Ce-OMS-2@CeO₂ catalyst. In the presence of SO₂ and H₂O, SO₂ could easily react with NH₃ and H₂O to produce ammonium bisulfate (NH₄HSO₄, ABS) on the surface of the Ce-OMS-2 and CeO₂/Ce-OMS-2 catalysts. Then ABS can be physically deposited on the surface of the catalysts, thus blocking the active Mn sites to participate in the SCR reaction. Interesting, for the core-shell Ce-OMS-2@CeO₂ catalyst, the formed ABS could significantly be decomposed at low temperature, leading to the exposure of surface active Mn sites of the catalyst. Herein, it could maintain the efficient SCR performance over the Ce-OMS-2@CeO₂ catalyst. A dynamic balance of ABS formation and decomposition was achieved over Ce-OMS-2@CeO₂ even at low temperatures, which hindered the SO₂ poisoning during the NH₃-SCR reaction. As expected, the core-shell Ce-OMS-2@CeO₂ catalyst showed excellent SCR performance and SO₂+H₂O resistance (~100% NO conversion in the temperature range of 100–200 °C without SO₂, ~80% NO conversion for 4 h in the presence of SO₂). This work provides an effective strategy for the development of efficient and stable Mn-based low-temperature SCR catalysts.

在非电力行业中，开发具有高度抗二氧化硫和水（SO2+H2O）性能的氮氧化物（NOx）低温选择性催化还原（SCR）催化剂是一项挑战。本文成功制备了核壳和负载型 Ce-OMS-2 复合物（Ce-OMS-2@CeO2 和 CeO2/Ce-OMS-2）。本文成功制备了核壳型和负载型 Ce-OMS-2 复合物（Ce-OMS-2@CeO2 和 CeO2/Ce-OMS-2），并对其质构特性和催化性能进行了表征。结果表明，核壳 Ce-OMS-2@CeO2 材料可以保持介孔结构，显著改善反应气体 NO 的传质和吸附，从而提高 SCR 效率。相反，对于负载了 CeO2/Ce-OMS-2 的催化剂，大量 CeO2 沉积在 Ce-OMS-2 表面，阻塞了介孔结构。此外，二氧化硫与 CeO2/Ce-OMS-2 反应生成大量金属硫酸盐（硫酸锰或硫酸铈），导致活性锰位点失活。因此，CeO2/Ce-OMS-2 催化剂在 SCR 反应中表现出较低的 SCR 活性和较差的 SO2+H2O 耐受性。我们还阐明了核壳 Ce-OMS-2@CeO2 催化剂抗硫的原因。在 SO2 和 H2O 的存在下，SO2 很容易与 NH3 和 H2O 反应，在 Ce-OMS-2 和 CeO2/Ce-OMS-2 催化剂表面生成硫酸氢铵（NH4HSO4，ABS）。然后，ABS 可以物理沉积在催化剂表面，从而阻断活性 Mn 位点参与 SCR 反应。有趣的是，对于核壳 Ce-OMS-2@CeO2 催化剂来说，形成的 ABS 在低温下就能显著分解，从而使催化剂表面活性锰位点暴露出来。因此，Ce-OMS-2@CeO2 催化剂可以保持高效的 SCR 性能。即使在低温条件下，Ce-OMS-2@CeO2 上也能实现 ABS 生成和分解的动态平衡，从而阻碍了 NH3-SCR 反应过程中的 SO2 中毒。正如预期的那样，核壳 Ce-OMS-2@CeO2 催化剂表现出优异的 SCR 性能和抗 SO2+H2O 性能（在无 SO2 的 100-200 °C 温度范围内，NO 转化率约为 100%；在有 SO2 存在的情况下，4 小时的 NO 转化率约为 80%）。这项工作为开发高效、稳定的锰基低温 SCR 催化剂提供了一种有效的策略。

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引用次数: 0

The effects of calcination temperature and dispersants on the catalytic performance of Co0.8Cu0.2/CNC for the hydrolysis of ammonia borane to hydrogen 煅烧温度和分散剂对 Co0.8Cu0.2/CNC 催化硼烷氨水解制氢性能的影响

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60462-7

Rong LI , Youhua ZUO , Licheng XU , Junfeng HUA , Jiajia FENG , Lixin XU , Mingfu YE , Chao WAN

Ammonia borane (NH₃BH₃, AB) is considered as an ideal hydrogen storage material for portable hydrogen production. In this paper, a bimetallic carbon cube (Co_0.8Cu_0.2/CNC) catalyst was prepared by high-temperature calcination of the Co_0.8Cu_0.2-ZIF precursor, which was obtained by stirring the reactants at room temperature. In addition, the microstructure and composition of the catalyst were investigated using various characterization methods. The change regularity of the catalyst was explored through the single-variable method. The results showed that the addition of a small amount of Cu had a stabilizing effect on the cubic morphology of the Co_0.8Cu_0.2/CNC catalyst. When the dispersant was CTAB and the calcination temperature was 873 K, the activation energy (E_a) for catalyzing the hydrolysis of AB to hydrogen was 50.79 kJ/mol with the transition frequency (TOF) value as high as 23.37 min^–1. Moreover, the catalyst could still catalyze the complete hydrolysis of AB to hydrogen after 25 cycles, which indicated that the catalyst had good stability performance.

氨硼烷（NH3BH3，AB）被认为是一种理想的储氢材料，可用于便携式制氢。本文通过对室温下搅拌反应物得到的 Co0.8Cu0.2-ZIF 前驱体进行高温煅烧，制备了双金属碳立方体（Co0.8Cu0.2/CNC）催化剂。此外，还使用各种表征方法研究了催化剂的微观结构和组成。通过单变量法探讨了催化剂的变化规律。结果表明，添加少量的 Cu 对 Co0.8Cu0.2/CNC 催化剂的立方形态有稳定作用。当分散剂为 CTAB，煅烧温度为 873 K 时，催化 AB 水解为氢气的活化能（Ea）为 50.79 kJ/mol，过渡频率（TOF）值高达 23.37 min-1。此外，催化剂在循环 25 次后仍能催化 AB 完全水解为氢气，这表明催化剂具有良好的稳定性能。

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引用次数: 0

Preparation of Ni/ZnCo2O4@ZnO composite metal oxide adsorbent and its adsorption desulfurization and regeneration performance Ni/ZnCo2O4@ZnO 复合金属氧化物吸附剂的制备及其吸附脱硫和再生性能

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60463-9

Pu DAI , Mengya GUO , Hui GE , Caimei FAN , Xuekuan LI , Rui LI , Mingxing TANG

Metal Co was introduced into ZnO by co-precipitation to form composite metal oxides as the desulfurization agent with different Co contents, with which the desulfurization activity and regeneration performance were investigated. The systematic characterization of the structure and properties of the desulfurization agent using XRD, TEM, N₂ adsorption and desorption, XPS and H₂-TPR confirmed that the composite metal oxide desulfurization agent had the Ni/ZnCo₂O₄@ZnO structure. The formation of ZnCo₂O₄ in the composite metal oxides desulfurization agent facilitated the particle size reduction, dispersion enhancement and specific surface area increase of the desulfurization agent, which also acted as an adsorbent for H₂S indicated by the XRD analysis, improving the sulfur adsorption capacity of the desulfurization agent. The desulfurization performance of all the composite metal oxide desulfurization agents was higher than that of Ni/ZnO, in which the desulfurization agent NZCo-3 with a molar ratio of Zn:Co of 1:1 exhibited the optimal desulfurization performance, and the desulfurization rate was 100% at a reaction temperature of 300 °C, a hydrogen pressure of 3 MPa, a mass-air velocity of 2.2 h^–1, and a hydrogen-oil ratio of 300, and the excellent desulfurization performance was maintained after 6 cycles. The results of this study provide new ideas for the rational design of Ni/ZnO desulfurization agent to improve its desulfurization and regeneration performance.

通过共沉淀将金属 Co 引入 ZnO 中，形成不同 Co 含量的复合金属氧化物作为脱硫剂，并研究了其脱硫活性和再生性能。利用 XRD、TEM、N2 吸附和解吸、XPS 和 H2-TPR 对脱硫剂的结构和性能进行了系统表征，证实复合金属氧化物脱硫剂具有 Ni/ZnCo2O4@ZnO 结构。复合金属氧化物脱硫剂中 ZnCo2O4 的形成促进了脱硫剂粒径的减小、分散性的增强和比表面积的增加，XRD 分析表明，ZnCo2O4 也起到了吸附 H2S 的作用，提高了脱硫剂的硫吸附能力。所有复合金属氧化物脱硫剂的脱硫性能均高于 Ni/ZnO，其中 Zn:Co 摩尔比为 1:1 的脱硫剂 NZCo-3 的脱硫性能最佳，在反应温度为 300 ℃、氢气压力为 3 MPa、质量-空气速度为 2.2 h-1、氢油比为 300 的条件下，脱硫率为 100%，且 6 次循环后仍能保持良好的脱硫性能。该研究结果为合理设计 Ni/ZnO 脱硫剂以提高其脱硫和再生性能提供了新思路。

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引用次数: 0

In-situ photodeposition of co-catalyst Ni2P on CdS for photocatalytic conversion of ethanol for synergistic hydrogen production 在 CdS 上原位光沉积辅助催化剂 Ni2P，用于乙醇的光催化转化以协同制氢

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60493-7

Yiming LIU , Jingjing MIAO , Wanggang ZHANG , Aili WEI , Jian WANG

In this study, Ni₂P/CdS composites were constructed by depositing non-precious metal co-catalyst Ni₂P on a one-dimensional network of CdS using a simple in-situ photodeposition method. The prepared photocatalysts promoted the decomposition of ethanol into high-value-added products while generating hydrogen. The composite photoanodes loaded with the Ni₂P co-catalysts showed significantly higher ethanol conversion and hydrogen production in the visible light region, which was almost three times higher than that of pure CdS. The main products of photocatalytic ethanol production are acetaldehyde (AA) and 2,3-butanediol (2,3-BDA). Compared with CdS, the selectivity of the composite photocatalysts for converting ethanol to acetaldehyde was significantly improved (62% to 78%). Characterization of the prepared photocatalysts confirmed that the loading of Ni₂P co-catalysts on CdS not only broadened the optical region of the catalysts for trapping light but also effectively promoted the separation and transfer of charge carriers, which significantly improved the photocatalytic efficiency of ethanol conversion and hydrogen production in the catalysts. It has been proven through Electron Paramagnetic Resonance testing that loading a Ni₂P co-catalyst on CdS is beneficial for the adsorption of hydroxyethyl radicals (*CH(OH)CH₃), thereby further improving the selectivity of acetaldehyde. This study plays an important role in the rational design of composite catalyst structures and the introduction of co-catalysts to improve catalyst performance, promote green chemistry, advocate a low-carbon society, and promote sustainable development.

本研究采用简单的原位光沉积法，在一维 CdS 网络上沉积非贵金属助催化剂 Ni2P，从而构建了 Ni2P/CdS 复合材料。所制备的光催化剂可促进乙醇分解成高附加值产品，同时产生氢气。负载了 Ni2P 助催化剂的复合光阳极在可见光区域的乙醇转化率和产氢量显著提高，几乎是纯 CdS 的三倍。光催化乙醇生产的主要产物是乙醛（AA）和 2,3-丁二醇（2,3-BDA）。与 CdS 相比，复合光催化剂将乙醇转化为乙醛的选择性显著提高（从 62% 提高到 78%）。对所制备光催化剂的表征证实，在 CdS 上负载 Ni2P 助催化剂不仅拓宽了催化剂捕获光的光学区域，还有效促进了电荷载流子的分离和转移，从而显著提高了催化剂中乙醇转化和制氢的光催化效率。通过电子顺磁共振测试证明，在 CdS 上负载 Ni2P 助催化剂有利于羟乙基（*CH(OH)CH3）的吸附，从而进一步提高乙醛的选择性。该研究对于合理设计复合催化剂结构，引入助催化剂，提高催化剂性能，推动绿色化学发展，倡导低碳社会，促进可持续发展具有重要作用。

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引用次数: 0

Development of Nix/Mg1–x-MOF-74 for highly efficient CO2/N2 separation 开发用于高效 CO2/N2 分离的 Nix/Mg1-x-MOF-74

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60464-0

Xin ZHANG , Guoqiang LI , Mei HONG , Hongyan BAN , Lixia YANG , Xingchen LIU , Feng LI , Ekaterina Vladimirovna Matus , Congming LI , Lei LI

To enhance the separation selectivity of Mg-MOF-74 towards CO₂ in a CO₂/N₂ mixture, a series of Mg-MOF-74 and Ni_x/Mg_1–x-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper. It was found that the adsorption capacity of Mg-MOF-74 for CO₂ could be effectively increased by optimizing the amount of acetic acid. On this basis, the bimetal MOF-74 adsorbent was prepared by metal modification. The multi-component dynamic adsorption penetration analysis was utilized to examine the CO₂ adsorption capacity and CO₂/N₂ selectivity of the diverse adsorbent materials. The results showed that Ni_0.11/Mg_0.89-MOF-74 showed a CO₂ adsorption capacity of 7.02 mmol/g under pure CO₂ atmosphere and had a selectivity of 20.50 for CO₂/N₂ under 15% CO₂/85% N₂ conditions, which was 10.2% and 18.02% higher than that of Mg-MOF-74 respectively. Combining XPS, SEM and N₂ adsorption-desorption characterization analysis, it was attributed to the effect of the more stable unsaturated metal sites Ni into the Mg-MOF-74 on the pore structure and the synergistic interaction between the two metals. Density Functional Theory (DFT) simulations revealed that the synergistic interaction between modulated the electrostatic potential strength and gradient of the material, which was more favorable for the adsorption of CO₂ molecules with small diameters and large quadrupole moment. In addition, the Ni_0.11/Mg_0.89-MOF-74 showed commendable cyclic stability, underscoring its promising potential for practical applications.

为了提高 Mg-MOF-74 对 CO2/N2 混合物中二氧化碳的分离选择性，本文采用溶热合成法制备了一系列 Mg-MOF-74 和 Nix/Mg1-x-MOF-74 吸附剂。研究发现，通过优化醋酸的用量，可有效提高 Mg-MOF-74 对 CO2 的吸附能力。在此基础上，通过金属改性制备了双金属 MOF-74 吸附剂。利用多组分动态吸附渗透分析法考察了不同吸附材料的 CO2 吸附能力和 CO2/N2 选择性。结果表明，Ni0.11/Mg0.89-MOF-74 在纯二氧化碳气氛下的二氧化碳吸附容量为 7.02 mmol/g，在 15% CO2/85% N2 条件下对 CO2/N2 的选择性为 20.50，分别比 Mg-MOF-74 高出 10.2% 和 18.02%。结合 XPS、SEM 和 N2 吸附-解吸表征分析，这归因于 Mg-MOF-74 中更稳定的不饱和金属位点 Ni 对孔隙结构的影响以及两种金属之间的协同作用。密度泛函理论（DFT）模拟显示，两种金属之间的协同作用调节了材料的静电势强度和梯度，更有利于吸附直径小、四极矩大的 CO2 分子。此外，Ni0.11/Mg0.89-MOF-74 还表现出了值得称道的循环稳定性，突显了其在实际应用中的巨大潜力。

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引用次数: 0

Research on improving carbon oxidation by fluorine doping in carbon-assisted water electrolysis for hydrogen production 碳辅助水电解制氢中通过掺氟改善碳氧化的研究

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60474-3

Qi LIU , Yanqing DOU , Zhouting GONG , Shoujun LIU , Liangyu CHEN , Yuwen TAO , Jinfang LIU , Song Yang

Faced with the constraints of the “carbon peaking and carbon neutrality goals”, the electrolysis of water for hydrogen production has received significant attention. However, high energy consumption is one of the problems hindering the industrialization of the technology. A strategy for “sacrificial anode carbon-assisted electrolysis of water for hydrogen production” is thus proposed, which uses the carbon oxidation reaction (COR) instead of the oxygen evolution reaction (OER) to achieve a significant reduction in energy consumption. In particular, F-doped biochar (denoted as F-BC-850) was prepared using a simple two-step carbonization method. The structural properties were analyzed using XRD, SEM-EDS, thermogravimetric, XPS and other characterization techniques. The structure-activity relationship was elucidated by electrochemical tests. The results showed that the energy consumption in 0.5 mol/L H₂SO₄ solution at 10 mA/cm² was 57.9% of the conventional Pt sheet electrode. Characterization results showed that HF generated by the pyrolysis of ammonium fluoride etched the biochar and formed highly active C–F bonds, which improved the oxidation performance of carbon. The addition of F species changed the carbon structure, promoted the decomposition of H₂O molecules to *OH radicals, and thus increased the adsorption ability of carbon atoms for *OH radicals. This work can provide theoretical guidelines for the efficient production of H₂ by carbon-assisted electrolysis of water and high-quality utilization of biomass.

面对 "碳峰值和碳中和目标 "的制约，电解水制氢技术受到极大关注。然而，高能耗是阻碍该技术产业化的问题之一。因此，我们提出了一种 "牺牲阳极碳辅助电解水制氢 "的策略，利用碳氧化反应（COR）代替氧进化反应（OER），从而大幅降低能耗。具体而言，采用简单的两步碳化法制备了掺杂 F 的生物炭（记为 F-BC-850）。利用 XRD、SEM-EDS、热重、XPS 等表征技术分析了其结构特性。通过电化学测试阐明了结构与活性的关系。结果表明，在 0.5 mol/L H2SO4 溶液中，10 mA/cm2 的能耗是传统铂片电极的 57.9%。表征结果表明，氟化铵热解产生的 HF 蚀刻了生物炭，形成了高活性的 C-F 键，提高了炭的氧化性能。F 物种的加入改变了碳的结构，促进了 H2O 分子分解为 *OH 自由基，从而提高了碳原子对 *OH 自由基的吸附能力。这项工作可为碳辅助电解水高效生产 H2 和生物质的高质量利用提供理论指导。

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引用次数: 0

Non-thermal plasma-catalytic reforming of tar over Ni-based catalysts 在镍基催化剂上对焦油进行非热等离子催化重整

Q3 Energy

燃料化学学报

Pub Date : 2024-11-01 DOI: 10.1016/S1872-5813(24)60475-5

Jinchao HU , Tian CHANG , Mingyan XIAO , Tian ZHANG , Xue HE

In the process of biomass gasification to produce syngas (H₂/CO), the production of tar as a by-product causes environmental pollution and hinders the development of gasification technology. The combination of non-thermal plasma and nickel-based catalysts can take advantage of the low reaction temperature of plasma and the high selectivity of catalyst to transform tar into syngas. However, carbon deposition of nickel particles in the reforming process easily causes catalyst deactivation, so designing and modifying the catalyst to improve its carbon resistance is the key to solving the catalyst deactivation problem. In this paper, the deactivation mechanism of nickel-based catalysts in the non-thermal plasma-catalytic reforming of tar system, the design and modification of catalysts to improve their carbon resistance, the types of the non-thermal plasma reactor and its tar reforming mechanism, the synergistic effects of non-thermal plasma and catalysts are reviewed. The research prospect of non-thermal plasma-catalytic reforming of tar system is also discussed. This paper provides a reference for the design and development of nickel-based catalysts in the non-thermal plasma-catalytic reforming of tar system.

在生物质气化生产合成气（H2/CO）的过程中，副产品焦油的产生会造成环境污染，阻碍气化技术的发展。非热等离子体与镍基催化剂的结合可利用等离子体的低反应温度和催化剂的高选择性将焦油转化为合成气。然而，镍颗粒在转化过程中的碳沉积容易导致催化剂失活，因此设计和改造催化剂以提高其抗碳性能是解决催化剂失活问题的关键。本文综述了焦油非热等离子体催化重整体系中镍基催化剂的失活机理、提高催化剂耐碳性的设计与改性、非热等离子体反应器的类型及其焦油重整机理、非热等离子体与催化剂的协同效应。还讨论了焦油非热等离子体催化重整系统的研究前景。本文为焦油非热等离子体催化重整系统中镍基催化剂的设计和开发提供了参考。

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