Communications Chemistry
·
2022
·Vol. 5
·期 1
·1-8
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IF 7.211
Xu Jiacheng,Zhang Tiantian,Fang Shiyu,Li Jing,Wu Zuliang,Wang Wei,Zhu Jiali,Gao Erhao,Yao Shuiliang
Understanding of the roles of oxygen species at reducible metal oxide surfaces under real oxidation conditions is important to improve the performance of these catalysts. The present study addresses this issue by applying a combination of operando diffuse reflectance infrared Fourier transform spectroscopy with a temperature-programmed reaction cell and mass spectrometry to explore the behaviors of oxygen species during H 2 oxidation in a temperature range of 25–400 °C at β-MnO 2 surfaces. It is revealed that O 2 is dissociated simultaneously into terminal-type oxygen (M 2+ -O 2– ) and bridge-type oxygen (M + -O 2– -M + ) via adsorption at the Mn cation with an oxygen vacancy. O 2 adsorption is inhibited if the Mn cation is covered with terminal-adsorbed species (O, OH, or H 2 O). In a temperature range of 110–150 °C, OH at Mn cation becomes reactive and its reaction product (H 2 O) can desorb from the Mn cation, resulting in the formation of bare Mn cation for O 2 adsorption and dissociation. At a temperature above 150 °C, OH is reactive enough to leave bare Mn cation for O 2 adsorption and dissociation. These results suggest that bare metal cations with oxygen vacancies are important to improve the performance of reducible metal oxide catalysts.
研究领域:
催化化学
·
材料科学
·
表面科学
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Feihu Li,Zhipeng Wang,Jiabao Wang,Bowen Yang,Ziqiang Zhang,Ruiming Yang,Guangqiang Chen,Yeguang Zhang,Fang Fang,Peng Wang,Fangfang Liu,Zili Zhan
Tuned LIG microstructures via laser parameters for high-efficiency H 2 sensing. • Developed a LIG-based flexible electrochemical hydrogen sensor with a response/recovery time of 2.6 s/3.2 s. • The sensor exhibits high selectivity, flexibility, linearity and stability. • Employing MnO 2 as the cathode material enables reliable hydrogen detection under oxygen-free conditions. Laser-induced graphene (LIG) technology has become an ideal strategy for fabricating electrode materials due to its ability to produce flexible graphene substrates rapidly and scalably. In this work, a planar flexible electrochemical hydrogen gas sensor with a quasi-fuel-cell structure is designed, which is based on a composite membrane electrode of LIG/Nafion/MnO 2 . By adjusting laser parameters, a porous laser-induced graphene (LIGP) substrate with high specific surface area and high graphitization is controllably fabricated. On this basis, an anode with low Pt loading is constructed. In particular, the arrayed gas diffusion channels enable hydrogen to diffuse and distribute directly and efficiently to the electrode surface. Manganese dioxide (MnO 2 ) serves as the cathode active material for the reduction reaction, replacing the kinetically sluggish oxygen reduction reaction (ORR) in conventional systems, thereby eliminating the dependence on oxygen. The optimized LIGP sensor exhibits response and recovery times of merely 2.6 s and 3.2 s, respectively, with a sensitivity up to 5.98 nA/ppm and a limit of detection (LOD) of 0.83 ppm, alongside excellent selectivity, long-term stability, and mechanical flexibility. This study integrates laser processing technology, electrode material optimization, and device structural innovation to achieve low cost and high sensing performance, providing a new route for the development and mass fabrication of flexible hydrogen sensors. Download: Download high-res image (298KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiaqi Ruan,Ke Guo,Bin Wang,Xiao Li,Mengzhu Sun,Yilin Li,Mingkai Liu,Yong Hao,Hongguang Jin
CO 2 sorption-desorption kinetics fitting of Li 4 SiO 4 particles using power-law model • Validated model integrating Pd Ag membrane, CO 2 sorption, and SMR reaction kinetics • Achieved >99% CH 4 conversion and high-purity of H 2 /CO 2 via dual-separation synergy • Net solar-to-H 2 efficiency is enhanced to 35.2% via dual-separation solar reforming • Understood the enhanced CH 4 conversion mechanism in dual-product separation system Solar thermochemical hydrogen production is a promising approach for solar energy utilization and storage. Conventional steam methane reforming remains the dominant industrial H 2 production route, but its feasibility for producing low-carbon-footprint H 2 is constrained by high-temperature (>950 °C), high energy penalties associated with product separation, and high CO 2 emissions. Here, we propose a method of integrating mid-temperature (450–600 °C) concentrated solar energy-driven steam methane reforming with Pd Ag membrane for H 2 separation and Li 4 SiO 4 sorbent for in-situ CO 2 capture. Isothermal sorption-desorption experiments were carried out on synthesized K-doped Li 4 SiO 4 particles under varying temperatures and CO 2 concentrations, with the kinetics fitted by a power-law model. Moreover, a one-dimensional transient model of sorption-enhanced Pd Ag membrane reactor was validated by the fixed-bed experimental platform with a relative error of less than 2%. Systematic research based on multiphysics modeling demonstrates that the ordered conversion and synergy of H 2 and CO 2 can achieve multiple objectives of high conversion rates, significant temperature reduction, acquisition of high-purity H 2 , and decarbonization. The Pd Ag membrane and alternating Ni-catalyst/Li 4 SiO 4 sorbent maintain low H 2 /CO 2 partial pressures, driving the equilibrium toward near-complete methane conversion. Numerical results demonstrate that this method enables nearly complete conversion of CH 4 at a flow rate of 360 mL/min with simultaneous separation of high-purity H 2 at a significantly reduced temperature of 500 °C. The first-law thermodynamic, net solar-to-H 2 , and exergy efficiencies are enhanced to 70.9%, 35.2%, and 64.8%, respectively. The methane saving rate and CO 2 reduction rate are 14.4 and 39.5 g/h, respectively. Mid-temperature (450–600 °C) concentrated solar energy-driven steam methane reforming with Pd Ag membrane for H 2 separation and Li 4 SiO 4 sorbent for CO 2 in-situ capture. Download: Download high-res image (193KB) Download: Download full-size image
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Journal of Physical Chemistry C
·
2026
·Vol. 130
·期 31
·10940-10951
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IF 3.4
Li Qing,Yang Yuke,Li Huajing,Yang Yiwen,Ma Siyu,Su Qiuxing,Shi Yonghong,Li Yuangang
The
synergistic coupling of photocatalytic hydrogen production
with high-value-added organic conversion provides a new research direction
for the efficient use of solar energy and green chemical synthesis.
However, key challenges remain in the same catalytic system, such
as severe carrier recombination and difficulty in precisely controlling
the interfacial reaction pathways. To address these issues, we construct
CdS/TiO 2 heterojunction photocatalysts with Pt species
introduced by ion exchange and photodeposition. As a result, the Cd(Pt)S/TiO 2 –Pt composite photocatalyst is successfully prepared.
Under visible light irradiation, the catalyst achieves highly selective
conversion of 4-pyridinemethanol to the C–C coupling product
1, 2-di(4-pyridyl)-1,2-ethanediol, with a selectivity of 89.22%. Under
optimized reaction conditions, the maximum H 2 production
rate of the catalyst reaches 4.66 mmol·g –1 ·h –1 . Mechanistic studies show that the photogenerated
holes enriched on the surface of Cd(Pt)S drive the sp 3 C–H
dehydrogenation of 4-pyridinemethanol to form •CH(OH)C 5 H 4 N radicals, which then undergo radical coupling
to form new C–C bonds. Meanwhile, the photogenerated electrons
transfer through TiO 2 to the Pt active sites to participate
in hydrogen evolution. This study provides new insights into regulating
the selective conversion of radicals via interfacial electronic engineering
and designing photocatalytic coupled reaction systems.
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ADVANCED FUNCTIONAL MATERIALS
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2026
·
IF 19.9
Yushen Xiao,Junchen Wang,Tongxin Tang,Kai-Hang Ye,Jieyu Li,Shuilian Cheng,Wenhao Zou,Junwei Chen,Xiaoxin Chen,Haoxian Shao,Hengjun Xie,Shengsen Zhang,Yueping Fang,Changyu Liu,Songcan Wang,Shanqing Zhang
Traditional photoelectrochemical (PEC) water splitting generally involves the kinetically sluggish oxygen evolution reaction, which not only restricts the hydrogen evolution reaction but also yields oxygen with little economic value. Herein, a Nafion/TiO 2-x photoanode is designed for coupling the PEC glucose oxidation reaction (GOR) with hydrogen production. Benefiting from charge migration between the Nafion layer and TiO 2-x , this approach effectively suppresses non-radiative recombination caused by vacancy-related surface traps. It also induces band bending, thereby enhancing the directional separation of photo-generated charges. Compared to pristine TiO 2 , this photoanode exhibits a fivefold increase in photocurrent density, outstanding long-term stability, and an absorbed photon-to-current conversion efficiency of 100%. Furthermore, the glucose oxidation efficiency reaches 97.8%, with a Faradaic efficiency of 80% for the selective oxidation of glucose to the high-value-added product of glucaric acid. Concurrently, the Faradaic efficiency for hydrogen evolution at the cathode is 99%, enabling simultaneous high-value organic synthesis and hydrogen co-production. Moreover, the Nafion/TiO 2-x photoanode demonstrates ultra-low detection limits and linear response at ultra-low concentrations for photoelectrochemical sensing. This research offers novel insights for synergistically optimising biomass resource utilisation and clean energy production.
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Sustainability
·
2026
·Vol. 18
·期 7
·3416
·
IF 4.1
Xinna Li,Fang Huang,Xinxin Wang,Zexu Chi,Han Yu
The efficient removal of low-concentration antibiotics from wastewater is a persistent challenge. In this work, we enhance the performance of a W-BiVO4photoanode by modifying it with CoNi-based metal–organic framework nanosheets (CoNi-MOF), constructing a W-BiVO4@CoNi-MOFN composite. This integration markedly improves the separation and migration of photogenerated charge carriers. Consequently, the modified photoanode delivers a substantially higher photocurrent density of 3.92 mA cm−2at 1.23 VRHE, representing a 2.3-fold enhancement over the pristine W-BiVO4(1.74 mA cm−2). Furthermore, the photoelectrocatalytic (PEC) system employing the W-BiVO4@CoNi-MOFN photoanode demonstrates significantly superior degradation efficiency for low-concentration tetracycline compared to the system based on unmodified W-BiVO4. The performance enhancement is attributed to a dual mechanism. First, the CoNi-MOF modification optimizes the PEC performance of W-BiVO4, facilitating the generation of photogenerated holes and active oxidants. Second, the composite photoanode exhibits enhanced tetracycline adsorption via π–π stacking and hydrogen bonding, thereby promoting degradation kinetics. The photoanode also shows excellent reusability. Total organic carbon (TOC) analysis and biotoxicity tests confirm effective mineralization and reduced environmental toxicity. Furthermore, the system demonstrates promising concurrent cathodic hydrogen evolution. This work highlights the potential of the W-BiVO4@CoNi-MOFN-based PEC system for integrated wastewater treatment and hydrogen production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Haobo Wang,Jing Cao,Hetong Wu,Weifeng Yao,Hexing Li
Piezocatalysis offers a sustainable route for converting mechanical energy into chemical fuels, yet its development is hindered by the limited availability of efficient non-centrosymmetric piezoelectric materials. Herein, centrosymmetric SrZrO 3 (SZO), a classic high-k dielectric, is further activated for enhanced piezocatalytic H 2 evolution through hydrothermal synthesis followed by mild acid etching. Pristine SZO already exhibits measurable H 2 evolution under ultrasonic excitation despite a negligible/very weak SHG response, suggesting that localized defect-associated polarization may contribute to a baseline piezocatalytic activity. After mild acid etching, the treated sample (SZO_aw) shows markedly enhanced piezocatalytic H 2 evolution together with a more evident symmetry-breaking response, enhanced local electromechanical behavior, modified surface-potential characteristics, and near-surface structural distortion. Comparative characterization further indicates that the dominant bulk perovskite framework is preserved after treatment, while the enhancement cannot be explained solely by increased surface area or by a simple bulk-averaged defect increase. Under identical ultrasonic conditions, SZO_aw delivers an H 2 evolution rate of 12.02 mmol·g −1 ·h −1 , which is about 10 times that of commercial SrZrO 3 and 3.4 times that of pristine SZO. These results support that mild-acid-induced near-surface polar/structural modification is an important contributing factor to the enhanced piezocatalytic performance of centrosymmetric SrZrO 3 , providing a viable strategy for enhancing piezocatalytic activity in centrosymmetric dielectrics.
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APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Xiangchen Kong,Shijie Hong,Xuyang Dong,Panpan Jiang,Kaiyue Wang,Yuming Tian
Mild calcination preserves porous TiO 2 (B) nanosheets and tunes oxygen vacancies • Oxygen vacancies stabilize highly dispersed metallic Cu on TiO 2 (B) • Cu-Vo interfaces promote electron transfer and suppress charge recombination • Cu-TiO 2 (B)-200 reaches 7.92 mmol g -1 h -1 under AM 1.5 simulated sunlight TiO 2 (B) is a promising photocatalyst for solar-driven H 2 evolution, yet its performance is limited by rapid charge recombination and insufficient surface reduction sites. Herein, a vacancy-assisted strategy combining mild thermal treatment with in situ photodeposition is developed to construct highly dispersed metallic Cu species on TiO 2 (B) nanosheets. Calcination at 200 °C preserves the metastable TiO 2 (B) framework while generating an appropriate concentration of surface oxygen vacancies, which serve as preferential anchoring sites for Cu and promote strong electronic coupling at the Cu-TiO 2 (B) interface. Under air mass 1.5 simulated sunlight with methanol as a sacrificial agent, the optimized Cu-loaded TiO 2 (B) sample treated at 200 °C achieves an H 2 evolution rate of 7.92 mmol g -1 h -1 and retains stable activity over five consecutive cycles. Comprehensive structural and spectroscopic characterizations, together with first-principles calculations, demonstrate that oxygen-vacancy-mediated Cu anchoring strengthens metal-support electronic coupling, promotes directional charge transfer and carrier separation, and facilitates interfacial proton reduction. These results establish a mechanistic correlation among phase preservation, oxygen-vacancy regulation, Cu dispersion, and photocatalytic performance. This work provides a practical and cost-effective strategy for constructing efficient non-noble-metal interfaces on metastable oxide photocatalysts. Download: Download high-res image (204KB) Download: Download full-size image A mild defect-engineering strategy preserves the TiO 2 (B) framework while generating oxygen vacancies that stabilize highly dispersed metallic Cu species. The resulting Cu-Vo interfaces promote directional electron transfer, suppress charge recombination, and facilitate interfacial proton reduction, thereby enhancing photocatalytic H 2 evolution under AM 1.5 simulated sunlight.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
·
IF 4.4
Jing Yang,Guangyu Huang,Hengtong Xia,Wenzhong Yang
Co complex [(tpy-NH 2 ) 2 Co]Cl 2 was synthesized for the first time. • CdTeS QDs and Co-1 loading conditions maximize photocathode performance. • The photocathode achieves 82 μA cm −2 photocurrent density and sustains over 3 h. • The photocathode produces 2.9 μmol H₂ with a Faradaic efficiency of 92.5%. The initial construction of a photocathode utilized CdTeS quantum dots (QDs), leveraging their remarkable photoelectric efficiency and photostability. The Co-1-CdTeS-NiO photocathode was fabricated by depositing a porous mesh NiO film on conductive glass as the substrate, preparing CdTeS QDs via the hydrothermal method, and loading them onto the NiO film surface. A non-precious metal [(tpy-NH₂)₂Co]Cl₂ complex was synthesized to replace the precious metal Pt as a hydrogen evolution co-catalyst. When subjected to visible light irradiation with an applied bias voltage of −0.1 V (vs. NHE), the photocurrent density reached 82 μA cm −2 and remained stable at 80 μA cm −2 over a 3 h stability test. Simultaneously, the photocathode generated 1.8 μmol of hydrogen gas, achieving a Faraday efficiency of 92.5%, thereby showcasing its highly efficient photocatalytic capabilities. Download: Download high-res image (130KB) Download: Download full-size image
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ACTA PHYSICO-CHIMICA SINICA
·
2026
·
IF 13.5
Yongkang Liu,Shouxi Yu,Li Chen,Zhongliao Wang,Meiyu Zhang,Jinfeng Zhang
Covalent organic frameworks (COFs) are widely studied as photocatalysts for the hydrogen evolution reaction (HER), yet most design strategies target light absorption or charge separation rather than the H* desorption barrier at the catalytic site itself. We re-examine the problem from a bond-resolved view: the crystal orbital Hamilton population (COHP) is used to treat the occupancy of the N−H antibonding manifold as a quantitative descriptor of how strongly the imine nitrogen of a Schiff-base COF binds H*. Two pyrene-based COFs, PY-BD and PY-DHBD, are synthesized to test the descriptor. Adding two phenolic −OH groups to the dialdehyde linker raises the antibonding occupancy (ICOHP from −7.52 to −7.18 eV), weakens the N−H bond, and shifts Δ G H* from −0.22 to 0.04 eV, close to thermoneutrality. The visible-light H 2 -evolution rate accordingly rises from 450 to 1127 μmol g −1 h −1 , 2.5-fold the rate of PY-BD. The work places COHP-resolved antibonding occupancy alongside the d -band-centre framework familiar from metal catalysis as a quantitative descriptor for tuning HER on N-rich COF active sites. Grafting electron-donating phenolic –OH groups onto a pyrene-based COF raises the N-H antibonding-orbital occupancy for photocatalytic H 2 evolution under visible light. Download: Download high-res image (149KB) Download: Download full-size image
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Catalysis Science & Technology
·
2026
·
IF 4
Longbo Zhang,Jia Guo,Yanyan Wang,Ying Wang,Jie Li,Hongxing Wang,Chenglong Yu,Yanru Zhang,Jun He,Xianyu Meng,Zhuo Zhang,Tianbin Wu,Qingli Qian,Li Tan,Buxing Han
Homogeneously catalyzed ethanol synthesis from CO2 and H2 usually uses expensive, unstable and complex catalyst precursors, hindering their industrial viability. In this work, a homogeneous catalytic system consisting of economic and stable catalyst precursors (RuCl3·3H2O and CoCl2·6H2O), cocatalyst (LiI) and N-ethyl-2-pyrrolidone (NEP) solvent was designed to accelerate ethanol production via methanol homologation with CO2 and H2. After activation of the catalyst precursors at 200 °C with CO, the target reaction could proceed efficiently under mild conditions (170 °C), with top level reaction selectivity (64.9%) and much higher space time yield (STY) of ethanol (3.9 g L−1 h−1) compared to previous reports with Ru/Co catalysts. The impact of activation conditions, reaction conditions, and the catalytic mechanism of the reaction were studied by a series of control experiments. This method of ethanol production has the advantages of a stable and easily available catalyst, excellent performance, and easy separation and recycling of the catalyst, showing great potential for industrialization.
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SENSORS AND ACTUATORS B-CHEMICAL
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2026
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IF 8.3
Wei Wei,Jinxiao Liu,Xinying Lu,Xiaohong Xia,Yuwen Bao,Cong Ye,Xiaolin Wu,Yun Gao
The development of highly sensitive hydrogen sensors with low operating temperatures is crucial for the safe utilization of hydrogen. Practical operating environments demand not only high sensitivity but also immunity to both humidity fluctuations and interference from other reducing gases, especially CO. In this work, hierarchical architectures comprising WO 3 nanosheets (NS) assembled on WO 3 microspheres (M) is deliberately designed and successfully synthesized via a two-step solvothermal method. Subsequently, Pt is functionally loaded onto the surfaces, adopting various morphologies and serving multiple functions for H 2 sensing. Notably, the optimal operating temperature is reduced to 50 °C while achieving exceptional sensing characteristics: an ultrahigh response of 8372.2 toward 1200 H 2 , a swift 2 s response time, outstanding selectivity with immunity to CO interference, excellent humidity immunity, and robust long-term stability. The mechanism underlying the superior sensing capability is systematically investigated to elucidate the performance enhancement. This work presents a pioneering approach to constructing high-performance, anti-interference gas sensors through hierarchical architecture engineering, offering new insights into the design and application of advanced sensing materials.
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